S J Schaper, E Metwalli, M V Kaeppel, A Kriele, R Gilles, K N Raftopoulos, P Müller-Buschbaum
Morphology–Ionic Conductivity Relationship in Polymer–Titania Hybrid Electrolytes for Lithium-Ion Batteries Journal Article
In: ACS Applied Energy Materials, vol. 4, no. 12, pp. 13438–13443, 2021.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Morphology\textendashIonic Conductivity Relationship in Polymer\textendashTitania Hybrid Electrolytes for Lithium-Ion Batteries},
author = {S J Schaper and E Metwalli and M V Kaeppel and A Kriele and R Gilles and K N Raftopoulos and P M\"{u}ller-Buschbaum},
url = {https://doi.org/10.1021/acsaem.1c03393},
doi = {10.1021/acsaem.1c03393},
year = {2021},
date = {2021-12-14},
urldate = {2021-12-14},
journal = {ACS Applied Energy Materials},
volume = {4},
number = {12},
pages = {13438\textendash13443},
abstract = {The morphology and ionic conductivity of a high-molecular-weight polystyrene-block-poly(ethylene oxide) (PS-b-PEO) diblock copolymer (DBC) solid-state hybrid electrolyte, prepared entirely from solution, containing the lithium salt LiTFSI ([Li]/[EO] = 0.1) and titania (TiO2) nanoparticles (NP) were investigated at different temperatures. Structure investigation using small-angle X-ray scattering (SAXS) indicates a rupture of the DBC morphology upon increasing TiO2\textendashNP content, without a significant decrease in the ionic conductivity at high TiO2\textendashNP contents. A high number of unbound charge carriers in the hybrid DBC electrolyte, achieved by careful tuning of the materials’ ratios, is the most important contribution to a high ionic conductivity.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
C Cai, K Liu, Y Zhu, P Li, Q Wang, B Liu, S Chen, H Li, L Zhu, H Li, J Fu, Y Chen, E Pensa, J Hu, Y-R Lu, T-S Chan, E Cortes, M Liu
Optimizing hydrogen binding on Ru sites with RuCo alloy nanosheets for efficient alkaline hydrogen evolution Journal Article
In: Angewandte Chemie International Edition, vol. n/a, no. n/a, 2021, ISSN: 1433-7851.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Optimizing hydrogen binding on Ru sites with RuCo alloy nanosheets for efficient alkaline hydrogen evolution},
author = {C Cai and K Liu and Y Zhu and P Li and Q Wang and B Liu and S Chen and H Li and L Zhu and H Li and J Fu and Y Chen and E Pensa and J Hu and Y-R Lu and T-S Chan and E Cortes and M Liu},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202113664},
doi = {https://doi.org/10.1002/anie.202113664},
issn = {1433-7851},
year = {2021},
date = {2021-11-25},
urldate = {2021-11-25},
journal = {Angewandte Chemie International Edition},
volume = {n/a},
number = {n/a},
abstract = {Ruthenium (Ru)-based catalysts, with considerable performance and desirable cost, become highly concerned candidates to replace platinum (Pt) in alkaline hydrogen evolution reaction (HER). The hydrogen binding at Ru sites (Ru-H) is an important factor limiting the HER activity. Herein, density functional theory (DFT) simulations show that the essence of Ru-H binding energy is the strong interaction between the 4dz 2 orbital of Ru and 1s orbital of H. The charge transfer between Ru sites and substrates (Co and Ni) causes the appropriate downward shift of the 4dz 2 -band center of Ru, which results in a Gibbs free energy of 0.022 eV for H* in RuCo system, much decrease compared to 0.133 eV in pure Ru system. This theoretical prediction has been experimentally confirmed using RuCo alloy nanosheets (RuCo ANSs). They were prepared via fast co-precipitation method followed with a mild electrochemical reduction. Structure characterizations reveal that the Ru atoms are embed into Co substrate as isolated active sites with the planar symmetric and Z-direction asymmetric coordination structure, obtaining an optimal 4dz 2 modulated electronic structure. Hydrogen sensor and temperature program desorption (TPD) tests demonstrate the enhanced Ru-H interactions in RuCo ANSs than pure Ru nanoparticles. As a result, the RuCo ANSs reach an ultra-low overpotential of 10 mV at 10 mA/cm 2 and a Tafel slope of 20.6 mV/dec in 1 M KOH, outperforming that of the commercial Pt/C. This holistic work provides a new insight to promote alkaline HER by optimizing metal-H binding energy of active sites.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
J Yun, R Sagehashi, Y Sato, T Masuda, S Hoshino, H B Rajendra, K Okuno, A Hosoe, A S Bandarenka, N Yabuuchi
Nanosized and metastable molybdenum oxides as negative electrode materials for durable high-energy aqueous Li-ion batteries Journal Article
In: Proceedings of the National Academy of Sciences, vol. 118, no. 48, pp. e2024969118, 2021.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Nanosized and metastable molybdenum oxides as negative electrode materials for durable high-energy aqueous Li-ion batteries},
author = {J Yun and R Sagehashi and Y Sato and T Masuda and S Hoshino and H B Rajendra and K Okuno and A Hosoe and A S Bandarenka and N Yabuuchi},
url = {https://www.pnas.org/doi/abs/10.1073/pnas.2024969118},
doi = {doi:10.1073/pnas.2024969118},
year = {2021},
date = {2021-11-23},
urldate = {2021-11-23},
journal = {Proceedings of the National Academy of Sciences},
volume = {118},
number = {48},
pages = {e2024969118},
abstract = {The development of inherently safe energy devices is a key challenge, and aqueous Li-ion batteries draw large attention for this purpose. Due to the narrow electrochemical stable potential window of aqueous electrolytes, the energy density and the selection of negative electrode materials are significantly limited. For achieving durable and high-energy aqueous Li-ion batteries, the development of negative electrode materials exhibiting a large capacity and low potential without triggering decomposition of water is crucial. Herein, a type of a negative electrode material (i.e., LixNb2/7Mo3/7O2) is proposed for high-energy aqueous Li-ion batteries. LixNb2/7Mo3/7O2 delivers a large capacity of ∼170 mA ⋅ h ⋅ g−1 with a low operating potential range of 1.9 to 2.8 versus Li/Li+ in 21 m lithium bis(trifluoromethanesulfonyl)amide (LiTFSA) aqueous electrolyte. A full cell consisting of Li1.05Mn1.95O4/Li9/7Nb2/7Mo3/7O2 presents high energy density of 107 W ⋅ h ⋅ kg−1 as the maximum value in 21 m LiTFSA aqueous electrolyte, and 73% in capacity retention is achieved after 2,000 cycles. Furthermore, hard X-ray photoelectron spectroscopy study reveals that a protective surface layer is formed at the surface of the negative electrode, by which the high-energy and durable aqueous batteries are realized with LixNb2/7Mo3/7O2. This work combines a high capacity with a safe negative electrode material through delivering the Mo-based oxide with unique nanosized and metastable characters.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
E Keil, P Malevich, J Hauer
Achromatic frequency doubling of supercontinuum pulses for transient absorption spectroscopy Journal Article
In: Optics Express, vol. 29, no. 24, pp. 39042-39054, 2021.
Abstract | Links | Tags: Solid-Liquid
@article{nokey,
title = {Achromatic frequency doubling of supercontinuum pulses for transient absorption spectroscopy},
author = {E Keil and P Malevich and J Hauer},
url = {http://www.osapublishing.org/oe/abstract.cfm?URI=oe-29-24-39042},
doi = {10.1364/OE.442400},
year = {2021},
date = {2021-11-22},
urldate = {2021-11-22},
journal = {Optics Express},
volume = {29},
number = {24},
pages = {39042-39054},
abstract = {We present achromatic frequency doubling of supercontinuum pulses from a hollow core fiber as a technique for obtaining tunable ultrashort pulses in the near UV and blue spectral range. Pulse energies are stable on a 1.1\% level, averaged over 100 000 shots. By the use of conventional optics only, we compress a 0.2 \µJ pulse at a center wavelength of 475 nm to a pulse duration of 12 fs, as measured by X-FROG. We test the capabilities of the approach by employing the ASHG-pulses as a pump in a transient absorption experiment on \β-carotene in solution.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
A C D López, T Eggert, K Reuter, N G Hörmann
Static and dynamic water structures at interfaces: A case study with focus on Pt(111) Journal Article
In: The Journal of Chemical Physics, vol. 155, no. 19, pp. 194702, 2021.
Links | Tags: Solid-Liquid
@article{nokey,
title = {Static and dynamic water structures at interfaces: A case study with focus on Pt(111)},
author = {A C D L\'{o}pez and T Eggert and K Reuter and N G H\"{o}rmann},
url = {https://aip.scitation.org/doi/abs/10.1063/5.0067106},
doi = {10.1063/5.0067106},
year = {2021},
date = {2021-11-18},
urldate = {2021-11-18},
journal = {The Journal of Chemical Physics},
volume = {155},
number = {19},
pages = {194702},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
J Mahl, O Gessner, J V Barth, P Feulner, S Neppl
Strong Potential Gradients and Electron Confinement in ZnO Nanoparticle Films: Implications for Charge-Carrier Transport and Photocatalysis Journal Article
In: ACS Applied Nano Materials, vol. 4, no. 11, pp. 12213-12221, 2021.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Strong Potential Gradients and Electron Confinement in ZnO Nanoparticle Films: Implications for Charge-Carrier Transport and Photocatalysis},
author = {J Mahl and O Gessner and J V Barth and P Feulner and S Neppl},
url = {https://doi.org/10.1021/acsanm.1c02730},
doi = {10.1021/acsanm.1c02730},
year = {2021},
date = {2021-11-11},
journal = {ACS Applied Nano Materials},
volume = {4},
number = {11},
pages = {12213-12221},
abstract = {Zinc oxide (ZnO) nanomaterials are promising components for chemical and biological sensors and photocatalytic conversion and operate as electron collectors in photovoltaic technologies. Many of these applications involve nanostructures in contact with liquids or exposed to ambient atmosphere. Under these conditions, single-crystal ZnO surfaces are known to form narrow electron accumulation layers with few nanometer spatial penetration into the bulk. A key question is to what extent such pronounced surface potential gradients can develop in the nanophases of ZnO, where they would dominate the catalytic activity by modulating charge-carrier mobility and lifetimes. Here, we follow the temperature-dependent surface electronic structure of nanoporous ZnO with photoemission spectroscopy to reveal a sizable, spatially averaged downward band bending for the hydroxylated state and a conservative upper bound of \<6 nm for the spatial extent of the associated potential gradient. This nanoscale confinement of conduction-band electrons to the nanoparticle film surface is crucial for a microscopic understanding and further optimization of charge transport and photocatalytic function in complex ZnO nanomaterials.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
C Feng, F Wang, Z Liu, M Nakabayashi, Y Xiao, Q Zeng, J Fu, Q Wu, C Cui, Y Han, N Shibata, K Domen, I D Sharp, Y Li
A self-healing catalyst for electrocatalytic and photoelectrochemical oxygen evolution in highly alkaline conditions Journal Article
In: Nature Communications, vol. 12, no. 1, pp. 5980, 2021, ISSN: 2041-1723.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {A self-healing catalyst for electrocatalytic and photoelectrochemical oxygen evolution in highly alkaline conditions},
author = {C Feng and F Wang and Z Liu and M Nakabayashi and Y Xiao and Q Zeng and J Fu and Q Wu and C Cui and Y Han and N Shibata and K Domen and I D Sharp and Y Li},
url = {https://doi.org/10.1038/s41467-021-26281-0},
doi = {10.1038/s41467-021-26281-0},
issn = {2041-1723},
year = {2021},
date = {2021-10-13},
journal = {Nature Communications},
volume = {12},
number = {1},
pages = {5980},
abstract = {While self-healing is considered a promising strategy to achieve long-term stability for oxygen evolution reaction (OER) catalysts, this strategy remains a challenge for OER catalysts working in highly alkaline conditions. The self-healing of the OER-active nickel iron layered double hydroxides (NiFe-LDH) has not been successful due to irreversible leaching of Fe catalytic centers. Here, we investigate the introduction of cobalt (Co) into the NiFe-LDH as a promoter for in situ Fe redeposition. An active borate-intercalated NiCoFe-LDH catalyst is synthesized using electrodeposition and shows no degradation after OER tests at 10 mA cm−2 at pH 14 for 1000 h, demonstrating its self-healing ability under harsh OER conditions. Importantly, the presence of both ferrous ions and borate ions in the electrolyte is found to be crucial to the catalyst’s self-healing. Furthermore, the implementation of this catalyst in photoelectrochemical devices is demonstrated with an integrated silicon photoanode. The self-healing mechanism leads to a self-limiting catalyst thickness, which is ideal for integration with photoelectrodes since redeposition is not accompanied by increased parasitic light absorption.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
Y Wang, E-P Yao, L Wu, J Feldmann, J K Stolarczyk
A Multi-Layer Device for Light-Triggered Hydrogen Production from Alkaline Methanol Journal Article
In: Angewandte Chemie International Edition, vol. 60, no. 51, pp. 26694-26701, 2021, ISSN: 1433-7851.
Abstract | Links | Tags: Solid-Liquid
@article{nokey,
title = {A Multi-Layer Device for Light-Triggered Hydrogen Production from Alkaline Methanol},
author = {Y Wang and E-P Yao and L Wu and J Feldmann and J K Stolarczyk},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202109979},
doi = {https://doi.org/10.1002/anie.202109979},
issn = {1433-7851},
year = {2021},
date = {2021-10-13},
journal = {Angewandte Chemie International Edition},
volume = {60},
number = {51},
pages = {26694-26701},
abstract = {Abstract It usually requires high temperature and high pressure to reform methanol with water to hydrogen with high turnover frequency (TOF). Here we show that hydrogen can be produced from alkaline methanol on a light-triggered multi-layer system with a very high hydrogen evolution rate up to ca. 1 μmol s−1 under the illumination of a standard Pt-decorated carbon nitride. The system can achieve a remarkable TOF up to 1.8×106 moles of hydrogen per mole of Pt per hour under mild conditions. The total turnover number (TTN) of 470 000 measured over 38 hours is among the highest reported. The system does not lead to any COx emissions, hence it could feed clean hydrogen to fuel cells. In contrast to a slurry system, the proposed multi-layer system avoids particle aggregation and effectively uses light and Pt active sites. The performance is also attributed to the light-triggered reforming of alkaline methanol. This notable performance is a promising step toward practical light-driven hydrogen generation.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
H Saini, P Kallem, E Otyepková, F Geyer, A Schneemann, V Ranc, F Banat, R Zbořil, M Otyepka, R A Fischer, K Jayaramulu
Two-dimensional MOF-based liquid marbles: surface energy calculations and efficient oil–water separation using a ZIF-9-III@PVDF membrane Journal Article
In: Journal of Materials Chemistry A, vol. 9, no. 41, pp. 23651-23659, 2021, ISSN: 2050-7488.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Two-dimensional MOF-based liquid marbles: surface energy calculations and efficient oil\textendashwater separation using a ZIF-9-III@PVDF membrane},
author = {H Saini and P Kallem and E Otyepkov\'{a} and F Geyer and A Schneemann and V Ranc and F Banat and R Zbo\v{r}il and M Otyepka and R A Fischer and K Jayaramulu},
url = {http://dx.doi.org/10.1039/D1TA05835E},
doi = {10.1039/D1TA05835E},
issn = {2050-7488},
year = {2021},
date = {2021-09-30},
journal = {Journal of Materials Chemistry A},
volume = {9},
number = {41},
pages = {23651-23659},
abstract = {Superhydrophobic MOF-nanosheets assembled on the outside of an aqueous droplet form ‘liquid marbles’. A facile mechanochemical-based synthesis followed by ultrasonication was used to prepare two-dimensional superhydrophobic\textendasholeophilic MOF nanosheets of a Co2+-based zeolitic imidazolate framework, namely ZIF-9-III ([Co4(bIm)16] with bIm− = benzimidazolate). The resulting ZIF-9-III showed excellent hydrophobicity (advancing water contact angle of 144°) and oleophilicity (oil contact angle of ≈0°). The superhydrophobic behavior originated from its predominant outer (002) surface, which featured nanoscale corrugation caused by the exposed benzimidazole groups. This behavior was corroborated by inverse gas chromatography measurements to determine the surface energies of bulk exfoliated 2D ZIF-9-III nanosheets and 3D ZIF-9-I. Taking advantage of the unique surface properties, including low surface energy and good moisture stability, we prepared ZIF-9-III@PVDF (PVDF = polyvinylidene fluoride) membranes following the non-solvent induced phase inversion (NIPS) process. The resulting membranes were exploited in real-time oil/water separation and featured remarkably high adsorption capacity and anti-staining properties. Therefore, this work opens the door to developing new superhydrophobic MOF-based composite materials with permeant porosity, which may enable applications in self-cleaning membranes for oil\textendashwater separation.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
S Pratap, F Babbe, N S Barchi, Z Yuan, T Luong, Z Haber, T-B Song, J L Slack, C V Stan, N Tamura, C M Sutter-Fella, P Müller-Buschbaum
Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating Journal Article
In: Nature Communications, vol. 12, no. 1, pp. 5624, 2021, ISSN: 2041-1723.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Out-of-equilibrium processes in crystallization of organic-inorganic perovskites during spin coating},
author = {S Pratap and F Babbe and N S Barchi and Z Yuan and T Luong and Z Haber and T-B Song and J L Slack and C V Stan and N Tamura and C M Sutter-Fella and P M\"{u}ller-Buschbaum},
url = {https://doi.org/10.1038/s41467-021-25898-5},
doi = {10.1038/s41467-021-25898-5},
issn = {2041-1723},
year = {2021},
date = {2021-09-24},
journal = {Nature Communications},
volume = {12},
number = {1},
pages = {5624},
abstract = {Complex phenomena are prevalent during the formation of materials, which affect their processing-structure-function relationships. Thin films of methylammonium lead iodide (CH3NH3PbI3, MAPI) are processed by spin coating, antisolvent drop, and annealing of colloidal precursors. The structure and properties of transient and stable phases formed during the process are reported, and the mechanistic insights of the underlying transitions are revealed by combining in situ data from grazing-incidence wide-angle X-ray scattering and photoluminescence spectroscopy. Here, we report the detailed insights on the embryonic stages of organic-inorganic perovskite formation. The physicochemical evolution during the conversion proceeds in four steps: i) An instant nucleation of polydisperse MAPI nanocrystals on antisolvent drop, ii) the instantaneous partial conversion of metastable nanocrystals into orthorhombic solvent-complex by cluster coalescence, iii) the thermal decomposition (dissolution) of the stable solvent-complex into plumboiodide fragments upon evaporation of solvent from the complex and iv) the formation (recrystallization) of cubic MAPI crystals in thin film.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
A L Oechsle, J E Heger, N Li, S Yin, S Bernstorff, P Müller-Buschbaum
Correlation of Thermoelectric Performance, Domain Morphology and Doping Level in PEDOT:PSS Thin Films Post-Treated with Ionic Liquids Journal Article
In: Macromolecular Rapid Communications, vol. 42, no. 20, pp. 2100397, 2021, ISSN: 1022-1336.
Abstract | Links | Tags: Solid-Liquid
@article{nokey,
title = {Correlation of Thermoelectric Performance, Domain Morphology and Doping Level in PEDOT:PSS Thin Films Post-Treated with Ionic Liquids},
author = {A L Oechsle and J E Heger and N Li and S Yin and S Bernstorff and P M\"{u}ller-Buschbaum},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/marc.202100397},
doi = {https://doi.org/10.1002/marc.202100397},
issn = {1022-1336},
year = {2021},
date = {2021-09-07},
journal = {Macromolecular Rapid Communications},
volume = {42},
number = {20},
pages = {2100397},
abstract = {Abstract Ionic liquid (IL) post-treatment of poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) thin films with ethyl-3-methylimidazolium dicyanamide (EMIM DCA), allyl-3-methylimidazolium dicyanamide (AMIM DCA), and 1-ethyl-3-methylimidazolium tetracyanoborate (EMIM TCB) is compared. Doping level modifications of PEDOT are characterized using UV\textendashVis spectroscopy and directly correlate with the observed Seebeck coefficient enhancement. With conductive atomic force microscopy (c-AFM) the authors investigate changes in the topographic-current features of the PEDOT:PSS thin film surface due to IL treatment. Grazing incidence small-angle X-ray scattering (GISAXS) demonstrates the morphological rearrangement towards an optimized PEDOT domain distribution upon IL post-treatment, directly facilitating the interconductivity and causing an increased film conductivity. Based on these improvements in Seebeck coefficient and conductivity, the power factor is increased up to 236 µW m−1K−2. Subsequently, a model is developed indicating that ILs, which contain small, sterically unhindered ions with a strong localized charge, appear beneficial to boost the thermoelectric performance of post-treated PEDOT:PSS films.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
A-K Hatz, R Calaminus, J Feijoo, F Treber, J Blahusch, T Lenz, M Reichel, K Karaghiosoff, N M Vargas-Barbosa, B V Lotsch
Chemical Stability and Ionic Conductivity of LGPS-Type Solid Electrolyte Tetra-Li7SiPS8 after Solvent Treatment Journal Article
In: ACS Applied Energy Materials, vol. 4, no. 9, pp. 9932-9943, 2021.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Chemical Stability and Ionic Conductivity of LGPS-Type Solid Electrolyte Tetra-Li7SiPS8 after Solvent Treatment},
author = {A-K Hatz and R Calaminus and J Feijoo and F Treber and J Blahusch and T Lenz and M Reichel and K Karaghiosoff and N M Vargas-Barbosa and B V Lotsch},
url = {https://doi.org/10.1021/acsaem.1c01917},
doi = {10.1021/acsaem.1c01917},
year = {2021},
date = {2021-08-30},
journal = {ACS Applied Energy Materials},
volume = {4},
number = {9},
pages = {9932-9943},
abstract = {The large-scale production of solid-state batteries necessitates the development of alternative routes for processing air-sensitive thiophosphate-based solid electrolytes. To set a basis for this, we investigate the chemical stability and ionic conductivity of the LGPS-type lithium-ion conductor tetra-Li7SiPS8 (LiSiPS) processed with various organic solvents. We elucidate the nature of colorful polysulfides that arise during solvent treatment and trace back their origin to the dissolution of the Li3PS4-type amorphous side phase typically present in LiSiPS. We find that water and alcohols decompose LiSiPS by the nucleophilic attack into oxygen-substituted thiophosphates and thioethers and propose a reaction mechanism for the latter. Moreover, we confirm that quaternary thiophosphates can be recrystallized from MeOH solutions upon subsequent high-temperature treatment. Aprotic solvents with donor numbers smaller than 15 kcal mol\textendash1 are suitable for wet-processing quaternary thiophosphates because both the crystal structure of the electrolyte and a high ionic conductivity of \>1 mS cm\textendash1 are retained. Using anisole as a case study, we clarify that a residual water content of up to 800 ppm does not lead to a significant deterioration in the ionic conductivity when compared to dry solvents (≤5 ppm). Additionally, we observe a decrease in ionic conductivity with an increasing amount of the solvent residue, which depends not only on the donor number of the solvent but also on the vapor pressure and interactions between the solvent molecules and thiophosphate groups in the solid electrolyte. Thus, optimization of solvent-processing methods of thiophosphate electrolytes is a multifaceted challenge. This work provides transferable insights regarding the stability of LiSiPS against organic solvents that may enable competitive and large-scale thiophosphate-based solid electrolyte processing.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
A-K Hatz, I Moudrakovski, S Bette, M W Terban, M Etter, M Joos, N M Vargas-Barbosa, R E Dinnebier, B V Lotsch
Fast Water-Assisted Lithium Ion Conduction in Restacked Lithium Tin Sulfide Nanosheets Journal Article
In: Chemistry of Materials, vol. 33, no. 18, pp. 7337-7349, 2021, ISSN: 0897-4756.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Fast Water-Assisted Lithium Ion Conduction in Restacked Lithium Tin Sulfide Nanosheets},
author = {A-K Hatz and I Moudrakovski and S Bette and M W Terban and M Etter and M Joos and N M Vargas-Barbosa and R E Dinnebier and B V Lotsch},
url = {https://doi.org/10.1021/acs.chemmater.1c01755},
doi = {10.1021/acs.chemmater.1c01755},
issn = {0897-4756},
year = {2021},
date = {2021-08-25},
journal = {Chemistry of Materials},
volume = {33},
number = {18},
pages = {7337-7349},
abstract = {While two-dimensional (2D) materials may preserve some intrinsic properties of the corresponding layered bulk material, new characteristics arise from their pronounced anisotropy or confinement effects. Recently, exceptionally high ionic conductivities were discovered in 2D materials such as graphene oxide and vermiculite. Here, we report on the water-assisted fast conduction of lithium ions in restacked lithium tin sulfide nanosheets. Li0.8Sn0.8S2 exfoliates spontaneously in water and can be restacked into homogeneous films in which the lithium content is decreased, and a partial substitution of sulfur with hydroxyl groups takes place. Using a recursive supercell refinement approach in reciprocal space along with real-space pair distribution function analysis, we describe restacked lithium tin sulfide as a partially turbostratically disordered material composed of lithium-containing and lithium-depleted layers. In humid air, the material takes up multiple layers of water that coordinate lithium ions in the space between the layers, increasing the stacking distance and screening the interaction between lithium ions and the anionic layers. This results in a 1000-fold increase in ionic conductivity up to 47 mS cm\textendash1 at high humidities. Orientation-dependent impedance spectroscopy suggests a facile in-plane conduction and a hindered out-of-plane conduction. Pulsed field gradient nuclear magnetic resonance spectroscopy reveals a fast, simultaneous diffusion of a majority and a minority species for both 7Li and 1H, suggesting water-assisted lithium diffusion to be at play. This study enlarges the family of nanosheet-based ionic conductors and helps to rationalize the transport mechanism of lithium ions enabled by hydration in a nanoconfined 2D space.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
S A Watzele, L Katzenmeier, J P Sabawa, B Garlyyev, A S Bandarenka
Temperature dependences of the double layer capacitance of some solid/liquid and solid/solid electrified interfaces. An experimental study Journal Article
In: Electrochimica Acta, vol. 391, pp. 138969, 2021, ISSN: 0013-4686.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid, Solid-Solid
@article{,
title = {Temperature dependences of the double layer capacitance of some solid/liquid and solid/solid electrified interfaces. An experimental study},
author = {S A Watzele and L Katzenmeier and J P Sabawa and B Garlyyev and A S Bandarenka},
url = {https://www.sciencedirect.com/science/article/pii/S0013468621012597},
doi = {https://doi.org/10.1016/j.electacta.2021.138969},
issn = {0013-4686},
year = {2021},
date = {2021-07-30},
journal = {Electrochimica Acta},
volume = {391},
pages = {138969},
abstract = {This study investigates the influence of the temperature on the electrical double layer capacitance (CDL) of various materials, which are essential for fuel cells and solid-state Li-ion batteries. Electrochemical impedance spectroscopy is utilized to measure the CDL of polycrystalline Pt/aqueous electrolytes interfaces, cathode catalyst layers of polymer electrolyte membrane fuel cells (PEMFC), and Au or Li electrodes in contact with a solid-state electrolyte (SSE), a prime example for solid-state ionics. Our results show that within the investigated temperature ranges, the CDL decreases with an increase in the temperature for Pt electrodes in an aqueous acidic electrolyte. However, for SSE and PEMFC cathode catalyst layers, the CDL increases with temperature. The CDL behavior with the temperature of herein presented systems is important for understanding and modeling of the interface processes for renewable energy conversion systems such as fuel cells, water electrolyzers, and batteries.},
keywords = {Foundry Inorganic, Solid-Liquid, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
P I Scheurle, A Mähringer, A Biewald, A Hartschuh, T Bein, D D Medina
MOF-74(M) Films Obtained through Vapor-Assisted Conversion—Impact on Crystal Orientation and Optical Properties Journal Article
In: Chemistry of Materials, vol. 33, no. 15, pp. 5896-5904, 2021, ISSN: 0897-4756.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {MOF-74(M) Films Obtained through Vapor-Assisted Conversion\textemdashImpact on Crystal Orientation and Optical Properties},
author = {P I Scheurle and A M\"{a}hringer and A Biewald and A Hartschuh and T Bein and D D Medina},
url = {https://doi.org/10.1021/acs.chemmater.1c00743},
doi = {10.1021/acs.chemmater.1c00743},
issn = {0897-4756},
year = {2021},
date = {2021-07-28},
journal = {Chemistry of Materials},
volume = {33},
number = {15},
pages = {5896-5904},
abstract = {In recent years, metal\textendashorganic frameworks (MOFs) with the structure MOF-74 have attracted much interest owing to their tunable pore aperture, high surface area, and electrical conductivity. The synthesis of well-defined, highly crystalline thin films of MOF-74 is of paramount importance for their implementation into device-based applications such as in chemical sensing, optoelectronics, gas storage, and separations. Here, we present the synthesis of highly crystalline MOF-74 (M = Zn2+, Mg2+, Ni2+, and Co2+) films by vapor-assisted conversion. MOF-74(M) thin films were grown on bare glass, quartz, gold, and silicon surfaces, showing high crystallinity, crystal orientation, and average thicknesses of 500 nm. By including a benzoic acid modulator, oriented MOF-74(Zn) films, with the crystallographic c-axis of the MOF crystallites oriented horizontally to the surface, were obtained on all substrates. In addition, highly crystalline MOF-74(Mg) was grown on glass and gold substrates with the crystallographic c-axis aligned orthogonally to the surface. Moreover, randomly oriented highly crystalline MOF-74(Co) and MOF-74(Ni) films were synthesized on glass, quartz, gold, and silicon. The pore accessibility of the obtained films was examined by means of krypton sorption measurements, revealing permanent and accessible porosity, reaching a BET surface area of 975 cm2/cm2 for MOF-74(Mg). Steady-state and time-resolved photoluminescence studies show emission in the blue spectral region of MOF-74(Zn and Mg) on quartz with a biexponential decay. In addition, confocal photoluminescence mapping confirmed a homogeneous MOF film surface with a similar emission profile over the whole examined area of 70 μm × 70 μm.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
M Joos, C Schneider, A Münchinger, I Moudrakovski, R Usiskin, J Maier, B V Lotsch
Impact of hydration on ion transport in Li2Sn2S5·xH2O Journal Article
In: Journal of Materials Chemistry A, vol. 9, no. 30, pp. 16532-16544, 2021, ISSN: 2050-7488.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Impact of hydration on ion transport in Li2Sn2S5·xH2O},
author = {M Joos and C Schneider and A M\"{u}nchinger and I Moudrakovski and R Usiskin and J Maier and B V Lotsch},
url = {http://dx.doi.org/10.1039/D1TA04736A},
doi = {10.1039/D1TA04736A},
issn = {2050-7488},
year = {2021},
date = {2021-07-23},
journal = {Journal of Materials Chemistry A},
volume = {9},
number = {30},
pages = {16532-16544},
abstract = {This work investigates the structure and transport properties of the layered material Li2Sn2S5·xH2O. The anhydrous phase shows a room-temperature Li+ diffusivity below 10−9 cm2 s−1 and conductivity below 10−5 S cm−1. Upon exposure to humidity, water intercalates between the layers and increases the interlayer distance, inducing first-order transitions to a hydrated phase (x ≈ 2\textendash4) and then to a second hydrated phase (x ≈ 8\textendash10). The latter is soft and sticky but remains solid. Diffusion of both Li+ ions and H2O remains predominantly two-dimensional under all conditions. The Li+ diffusivity and conductivity both increase by three orders of magnitude upon hydration, reaching values of 5 × 10−7 cm2 s−1 and 10−2 S cm−1 in the second hydrate. These transport rates are extraordinary for a solid electrolyte and approach what is typically seen in aqueous solutions. The material Li2Sn2S5·xH2O thus bridges the gap between a hydrated solid electrolyte and a confined liquid electrolyte, which is scientifically interesting and potentially useful in battery applications. In the light of these findings, a previous work on Li2Sn2S5 from our groups is revisited.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
K Jayaramulu, M Esclance Dmello, K Kesavan, A Schneemann, M Otyepka, S Kment, C Narayana, S B Kalidindi, R S Varma, R Zboril, R A Fischer
A multifunctional covalently linked graphene–MOF hybrid as an effective chemiresistive gas sensor Journal Article
In: Journal of Materials Chemistry A, vol. 9, no. 32, pp. 17434-17441, 2021, ISSN: 2050-7488.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {A multifunctional covalently linked graphene\textendashMOF hybrid as an effective chemiresistive gas sensor},
author = {K Jayaramulu and M Esclance Dmello and K Kesavan and A Schneemann and M Otyepka and S Kment and C Narayana and S B Kalidindi and R S Varma and R Zboril and R A Fischer},
url = {http://dx.doi.org/10.1039/D1TA03246A},
doi = {10.1039/D1TA03246A},
issn = {2050-7488},
year = {2021},
date = {2021-07-22},
journal = {Journal of Materials Chemistry A},
volume = {9},
number = {32},
pages = {17434-17441},
abstract = {A hybrid of GA@UiO-66-NH2 was synthesized based on the covalent assembly of graphene acid (GA) and the amine functionalized UiO-66 metal\textendashorganic framework through amide bonds. This strategy endows the material with unique properties, such as hierarchical pores, a porous conductive network decorated with functional groups, a high specific surface area, and a good chemical and thermal stability. The resultant hybrid has an electrical resistance of ∼104 Ω, whereas the pristine GA and UiO-66-NH2 possess an electrical resistance of ∼102 Ω and ∼109 Ω, respectively. The hybrid GA@UiO-66-NH2 was demonstrated for CO2 chemiresistive sensing and displayed a very fast response and quick recovery time of ∼18 s for 100% CO2, at 200 °C. While the pristine GA exhibits negligible response under the same conditions, GA@UiO-66-NH2 exhibited a response of 10 ± 0.6%. Further, in situ temperature dependent Raman studies during CO2 exposure confirm the presence of strong hydrogen bonding interaction between CO2 and the amide functionality present on GA@UiO-66-NH2. The resulting gas sensing characteristics of GA@UiO-66-NH2 are majorly attributed to the better interaction of CO2 at the amide/amine functional groups and the readily accessible hierarchical pores. This design strategy opens new horizons in the development of covalently linked hybrids with hierarchical porous conductive networks which can help to improve the gas sensing properties of MOF-based materials.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
S Hou, R M Kluge, R W Haid, E L Gubanova, S A Watzele, A S Bandarenka, B Garlyyev
In: ChemElectroChem, vol. 8, no. 18, pp. 3433-3456, 2021, ISSN: 2196-0216.
Abstract | Links | Tags: Solid-Liquid
@article{nokey,
title = {A Review on Experimental Identification of Active Sites in Model Bifunctional Electrocatalytic Systems for Oxygen Reduction and Evolution Reactions},
author = {S Hou and R M Kluge and R W Haid and E L Gubanova and S A Watzele and A S Bandarenka and B Garlyyev},
url = {https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/celc.202100584},
doi = {https://doi.org/10.1002/celc.202100584},
issn = {2196-0216},
year = {2021},
date = {2021-07-08},
urldate = {2021-07-08},
journal = {ChemElectroChem},
volume = {8},
number = {18},
pages = {3433-3456},
abstract = {Abstract Efficient electrocatalysis of the oxygen reduction (ORR) and evolution (OER) reactions is essential in numerous renewable energy conversion systems, such as fuel cells, metal-air batteries, and water electrolyzers. Design and optimization of electrocatalytic materials for such systems primarily rely on understanding the nature of active centers on the catalyst surface. This review focuses on several important aspects of the experimental identification of active sites on various model bifunctional ORR/OER electrocatalytic surfaces. Applications of the state-of-the-art experimental techniques are analyzed. In addition, approaches to investigate and understand the influence of some supporting electrolyte components on the ORR and OER activities are discussed.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
S Xue, R W Haid, R M Kluge, X Ding, B Garlyyev, J Fichtner, S Watzele, S J Hou, A S Bandarenka
Enhancing the Hydrogen Evolution Reaction Activity of Platinum Electrodes in Alkaline Media Using Nickel-Iron Clusters Journal Article
In: Angewandte Chemie-International Edition, vol. 59, no. 27, pp. 10934-10938, 2021, ISSN: 1433-7851.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Enhancing the Hydrogen Evolution Reaction Activity of Platinum Electrodes in Alkaline Media Using Nickel-Iron Clusters},
author = {S Xue and R W Haid and R M Kluge and X Ding and B Garlyyev and J Fichtner and S Watzele and S J Hou and A S Bandarenka},
url = {\<Go to ISI\>://WOS:000529657400001},
doi = {10.1002/anie.202000383},
issn = {1433-7851},
year = {2021},
date = {2021-06-18},
urldate = {2020-06-26},
journal = {Angewandte Chemie-International Edition},
volume = {59},
number = {27},
pages = {10934-10938},
abstract = {Herein, we demonstrate an easy way to improve the hydrogen evolution reaction (HER) activity of Pt electrodes in alkaline media by introducing Ni-Fe clusters. As a result, the overpotential needed to achieve a current density of 10 mA cm(-2) in H-2-saturated 0.1 m KOH is reduced for the model single-crystal electrodes down to about 70 mV. To our knowledge, these modified electrodes outperform any other reported electrocatalysts tested under similar conditions. Moreover, the influence of 1) Ni to Fe ratio, 2) cluster coverage, and 3) the nature of the alkali-metal cations present in the electrolyte on the HER activity has been investigated. The observed catalytic performance likely originates from both the improved water dissociation at the Ni-Fe clusters and the subsequent optimal hydrogen adsorption and recombination at Pt atoms present at the Ni-Fe/Pt boundary.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
X Ding, B Garlyyev, S A Watzele, T Kobina Sarpey, A S Bandarenka
Spotlight on the Effect of Electrolyte Composition on the Potential of Maximum Entropy: Supporting Electrolytes Are Not Always Inert Journal Article
In: Chemistry – A European Journal, vol. 27, no. 39, pp. 10016-10020, 2021, ISSN: 0947-6539.
Abstract | Links | Tags: Solid-Liquid
@article{nokey,
title = {Spotlight on the Effect of Electrolyte Composition on the Potential of Maximum Entropy: Supporting Electrolytes Are Not Always Inert},
author = {X Ding and B Garlyyev and S A Watzele and T Kobina Sarpey and A S Bandarenka},
url = {https://chemistry-europe.onlinelibrary.wiley.com/doi/abs/10.1002/chem.202101537},
doi = {https://doi.org/10.1002/chem.202101537},
issn = {0947-6539},
year = {2021},
date = {2021-05-29},
urldate = {2021-05-29},
journal = {Chemistry \textendash A European Journal},
volume = {27},
number = {39},
pages = {10016-10020},
abstract = {Abstract The influence of electrolyte pH, the presence of alkali metal cations (Na+, K+), and the presence of O2 on the interfacial water structure of polycrystalline gold electrodes has been experimentally studied in detail. The potential of maximum entropy (PME) was determined by the laser-induced current transient (LICT) technique. Our results demonstrate that increasing the electrolyte pH and introducing O2 shift the PME to more positive potentials. Interestingly, the PME exhibits a higher sensitivity to the pH change in the presence of K+ than Na+. Altering the pH of the K2SO4 solution from 4 to 6 can cause a drastic shift in the PME. These findings reveal that, for example, K2SO4 and Na2SO4 cannot be considered as equal supporting electrolytes: it is not a viable assumption. This can likely be extrapolated to other common “inert” supporting electrolytes. Beyond this, knowledge about the near-ideal electrolyte composition can be used to optimize electrochemical devices such as electrolyzers, fuel cells, batteries, and supercapacitors.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
P M Stanley, J Haimerl, C Thomas, A Urstoeger, M Schuster, N B Shustova, A Casini, B Rieger, J Warnan, R A Fischer
Host–Guest Interactions in a Metal–Organic Framework Isoreticular Series for Molecular Photocatalytic CO2 Reduction Journal Article
In: Angewandte Chemie International Edition, vol. 60, no. 33, pp. 17854-17860, 2021, ISSN: 1433-7851.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Host\textendashGuest Interactions in a Metal\textendashOrganic Framework Isoreticular Series for Molecular Photocatalytic CO2 Reduction},
author = {P M Stanley and J Haimerl and C Thomas and A Urstoeger and M Schuster and N B Shustova and A Casini and B Rieger and J Warnan and R A Fischer},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202102729},
doi = {https://doi.org/10.1002/anie.202102729},
issn = {1433-7851},
year = {2021},
date = {2021-05-20},
journal = {Angewandte Chemie International Edition},
volume = {60},
number = {33},
pages = {17854-17860},
abstract = {Abstract A strategy to improve homogeneous molecular catalyst stability, efficiency, and selectivity is the immobilization on supporting surfaces or within host matrices. Herein, we examine the co-immobilization of a CO2 reduction catalyst [ReBr(CO)3(4,4′-dcbpy)] and a photosensitizer [Ru(bpy)2(5,5′-dcbpy)]Cl2 using the isoreticular series of metal\textendashorganic frameworks (MOFs) UiO-66, -67, and -68. Specific host pore size choice enables distinct catalyst and photosensitizer spatial location\textemdasheither at the outer MOF particle surface or inside the MOF cavities\textemdashaffecting catalyst stability, electronic communication between reaction center and photosensitizer, and consequently the apparent catalytic rates. These results allow for a rational understanding of an optimized supramolecular layout of catalyst, photosensitizer, and host matrix.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
J Eichhorn, C-M Jiang, J K Cooper, I D Sharp, F M Toma
Nanoscale Heterogeneities and Composition–Reactivity Relationships in Copper Vanadate Photoanodes Journal Article
In: ACS Applied Materials & Interfaces, vol. 13, no. 20, pp. 23575-23583, 2021, ISSN: 1944-8244.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Nanoscale Heterogeneities and Composition\textendashReactivity Relationships in Copper Vanadate Photoanodes},
author = {J Eichhorn and C-M Jiang and J K Cooper and I D Sharp and F M Toma},
url = {https://doi.org/10.1021/acsami.1c01848},
doi = {10.1021/acsami.1c01848},
issn = {1944-8244},
year = {2021},
date = {2021-05-17},
urldate = {2021-05-17},
journal = {ACS Applied Materials \& Interfaces},
volume = {13},
number = {20},
pages = {23575-23583},
abstract = {The photoelectrochemical performance of thin film photoelectrodes can be impacted by deviations from the stoichiometric composition, both at the macroscale and at the nanoscale. This issue is especially pronounced for the class of ternary compounds that are currently investigated for simultaneously achieving the optoelectronic characteristics and chemical stability required for solar fuel generation. Here, we combine macroscopic photoelectrochemical testing with atomic force microscopy (AFM) and scanning transmission X-ray microscopy (STXM) to reveal relationships between photoelectrochemical activity, nanoscale morphology, and local chemical composition in copper vanadate (CVO) thin films as a model system. For films with varying Cu/(Cu + V) ratios around the ideal stoichiometry of stoiberite Cu5V2O10, AFM resolves submicrometer morphology variations, which correlate with variations of the Cu content resolved by STXM. Both stoichiometric and Cu-deficient films exhibit a clear photoresponse, which indicates electronic tolerance to reduced Cu content. While both films exhibit homogeneous O and V content, they are also characterized by local regions of Cu enrichment and depletion that extend beyond individual grains. By contrast, Cu-rich photoelectrodes exhibit a tendency toward CuO secondary phase formation and a significantly reduced photoelectrochemical activity, indicating a significantly poor electronic tolerance to Cu-enrichment. These findings highlight that the average film composition at the macroscale is insufficient for defining structure\textendashfunction relationships in complex ternary compounds. Rather, correlating microscopic variations in chemical composition to macroscopic photoelectrochemical performance provides insights into photocatalytic activity and stability that are otherwise not apparent from pure macroscopic characterization.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
L Zhu, Y Lin, K Liu, E Cortés, H Li, J Hu, A Yamaguchi, X Liu, M Miyauchi, J Fu, M Liu
Tuning the intermediate reaction barriers by a CuPd catalyst to improve the selectivity of CO2 electroreduction to C2 products Journal Article
In: Chinese Journal of Catalysis, vol. 42, no. 9, pp. 1500-1508, 2021, ISSN: 1872-2067.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Tuning the intermediate reaction barriers by a CuPd catalyst to improve the selectivity of CO2 electroreduction to C2 products},
author = {L Zhu and Y Lin and K Liu and E Cort\'{e}s and H Li and J Hu and A Yamaguchi and X Liu and M Miyauchi and J Fu and M Liu},
url = {https://www.sciencedirect.com/science/article/pii/S1872206720637548},
doi = {https://doi.org/10.1016/S1872-2067(20)63754-8},
issn = {1872-2067},
year = {2021},
date = {2021-05-12},
urldate = {2021-05-12},
journal = {Chinese Journal of Catalysis},
volume = {42},
number = {9},
pages = {1500-1508},
abstract = {Electrochemical CO2 reduction is a promising strategy for the utilization of CO2 and intermittent excess electricity. Cu is the only single metal catalyst that can electrochemically convert CO2 into multicarbon products. However, Cu exhibits an unfavorable activity and selectivity for the generation of C2 products because of the insufficient amount of CO* provided for the C-C coupling. Based on the strong CO2 adsorption and ultrafast reaction kinetics of CO* formation on Pd, an intimate CuPd(100) interface was designed to lower the intermediate reaction barriers and improve the efficiency of C2 product formation. Density functional theory (DFT) calculations showed that the CuPd(100) interface enhanced the CO2 adsorption and decreased the CO2* hydrogenation energy barrier, which was beneficial for the C-C coupling. The potential-determining step (PDS) barrier of CO2 to C2 products on the CuPd(100) interface was 0.61 eV, which was lower than that on Cu(100) (0.72 eV). Encouraged by the DFT calculation results, the CuPd(100) interface catalyst was prepared by a facile chemical solution method and characterized by transmission electron microscopy. CO2 temperature-programmed desorption and gas sensor experiments further confirmed the enhancement of the CO2 adsorption and CO2* hydrogenation ability of the CuPd(100) interface catalyst. Specifically, the obtained CuPd(100) interface catalyst exhibited a C2 Faradaic efficiency of 50.3% ± 1.2% at −1.4 VRHE in 0.1 M KHCO3, which was 2.1 times higher than that of the Cu catalyst (23.6% ± 1.5%). This study provides the basis for the rational design of Cu-based electrocatalysts for the generation of multicarbon products by fine-tuning the intermediate reaction barriers.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
F Zoller, S Häringer, D Böhm, J Luxa, Z Sofer, D Fattakhova-Rohlfing
Carbonaceous Oxygen Evolution Reaction Catalysts: From Defect and Doping-Induced Activity over Hybrid Compounds to Ordered Framework Structures Journal Article
In: Small, pp. e2007484, 2021, ISSN: 1613-6810.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Carbonaceous Oxygen Evolution Reaction Catalysts: From Defect and Doping-Induced Activity over Hybrid Compounds to Ordered Framework Structures},
author = {F Zoller and S H\"{a}ringer and D B\"{o}hm and J Luxa and Z Sofer and D Fattakhova-Rohlfing},
doi = {10.1002/smll.202007484},
issn = {1613-6810},
year = {2021},
date = {2021-05-04},
journal = {Small},
pages = {e2007484},
abstract = {Oxygen evolution reaction (OER) is expected to be of great importance for the future energy conversion and storage in form of hydrogen by water electrolysis. Besides the traditional noble-metal or transition metal oxide-based catalysts, carbonaceous electrocatalysts are of great interest due to their huge structural and compositional variety and unrestricted abundance. This review provides a summary of recent advances in the field of carbon-based OER catalysts ranging from "pure" or unintentionally doped carbon allotropes over heteroatom-doped carbonaceous materials and carbon/transition metal compounds to metal oxide composites where the role of carbon is mainly assigned to be a conductive support. Furthermore, the review discusses the recent developments in the field of ordered carbon framework structures (metal organic framework and covalent organic framework structures) that potentially allow a rational design of heteroatom-doped 3D porous structures with defined composition and spatial arrangement of doping atoms to deepen the understanding on the OER mechanism on carbonaceous structures in the future. Besides introducing the structural and compositional origin of electrochemical activity, the review discusses the mechanism of the catalytic activity of carbonaceous materials, their stability under OER conditions, and potential synergistic effects in combination with metal (or metal oxide) co-catalysts.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
R Lauenstein, S L Mader, H Derondeau, O Z Esezobor, M Block, A J Römer, C Jandl, E Riedle, V R I Kaila, J Hauer, E Thyrhaug, C R Hess
The central role of the metal ion for photoactivity: Zn– vs. Ni–Mabiq Journal Article
In: Chemical Science, 2021, ISSN: 2041-6520.
Abstract | Links | Tags: Molecularly-Functionalized, Solid-Liquid
@article{,
title = {The central role of the metal ion for photoactivity: Zn\textendash vs. Ni\textendashMabiq},
author = {R Lauenstein and S L Mader and H Derondeau and O Z Esezobor and M Block and A J R\"{o}mer and C Jandl and E Riedle and V R I Kaila and J Hauer and E Thyrhaug and C R Hess},
url = {http://dx.doi.org/10.1039/D0SC06096H},
doi = {10.1039/D0SC06096H},
issn = {2041-6520},
year = {2021},
date = {2021-04-21},
journal = {Chemical Science},
abstract = {Photoredox catalysts are integral components of artificial photosystems, and have recently emerged as powerful tools for catalysing numerous organic reactions. However, the development of inexpensive and efficient earth-abundant photoredox catalysts remains a challenge. We here present the photochemical and photophysical properties of a Ni\textendashMabiq catalyst ([NiII(Mabiq)]OTf (1); Mabiq = 2-4:6-8-bis(3,3,4,4-tetramethyldihydropyrrolo)-10-15-(2,2-biquinazolino)-[15]-1,3,5,8,10,14-hexaene1,3,7,9,11,14-N6)\textemdashand of a Zn-containing analogue ([ZnII(Mabiq)OTf] (2))\textemdashusing steady state and time resolved optical spectroscopy, time-dependent density functional theory (TDDFT) calculations, and reactivity studies. The Ni and Zn complexes exhibit similar absorption spectra, but markedly different photochemical properties. These differences arise because the excited states of 2 are ligand-localized, whereas metal-centered states account for the photoactivity of 1. The distinct properties of the Ni and Zn complexes are manifest in their behavior in the photo-driven aza-Henry reaction and oxidative coupling of methoxybenzylamine.},
keywords = {Molecularly-Functionalized, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
L V Besteiro, E Cortés, S Ishii, P Narang, R F Oulton
Hot electron physics and applications Journal Article
In: Journal of Applied Physics, vol. 129, no. 15, pp. 150401, 2021.
Links | Tags: Solid-Liquid, Solid-Solid
@article{,
title = {Hot electron physics and applications},
author = {L V Besteiro and E Cort\'{e}s and S Ishii and P Narang and R F Oulton},
url = {https://aip.scitation.org/doi/abs/10.1063/5.0050796},
doi = {10.1063/5.0050796},
year = {2021},
date = {2021-04-19},
journal = {Journal of Applied Physics},
volume = {129},
number = {15},
pages = {150401},
keywords = {Solid-Liquid, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
N G Hörmann, K Reuter
Thermodynamic Cyclic Voltammograms: Peak Positions and Shapes Journal Article
In: Journal of Physics: Condensed Matter, 2021, ISSN: 0953-8984.
Tags: Solid-Liquid
@article{,
title = {Thermodynamic Cyclic Voltammograms: Peak Positions and Shapes},
author = {N G H\"{o}rmann and K Reuter},
issn = {0953-8984},
year = {2021},
date = {2021-04-13},
urldate = {2021-04-13},
journal = {Journal of Physics: Condensed Matter},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
C Griesser, H Li, E-M Wernig, D Winkler, Shakibi N Nia, T Mairegger, T Götsch, T Schachinger, A Steiger-Thirsfeld, S Penner, D Wielend, D A Egger, C Scheurer, K Reuter, J Kunze-Liebhäuser
True Nature of the Transition-Metal Carbide/Liquid Interface Determines Its Reactivity Journal Article
In: ACS Catalysis, pp. 4920-4928, 2021.
Abstract | Links | Tags: Solid-Liquid
@article{,
title = {True Nature of the Transition-Metal Carbide/Liquid Interface Determines Its Reactivity},
author = {C Griesser and H Li and E-M Wernig and D Winkler and Shakibi N Nia and T Mairegger and T G\"{o}tsch and T Schachinger and A Steiger-Thirsfeld and S Penner and D Wielend and D A Egger and C Scheurer and K Reuter and J Kunze-Liebh\"{a}user},
url = {https://pubs.acs.org/doi/abs/10.1021/acscatal.1c00415},
doi = {10.1021/acscatal.1c00415},
year = {2021},
date = {2021-04-07},
urldate = {2021-04-07},
journal = {ACS Catalysis},
pages = {4920-4928},
abstract = {Compound materials, such as transition-metal (TM) carbides, are anticipated to be effective electrocatalysts for the carbon dioxide reduction reaction (CO2RR) to useful chemicals. This expectation is nurtured by density functional theory (DFT) predictions of a break of key adsorption energy scaling relations that limit CO2RR at parent TMs. Here, we evaluate these prospects for hexagonal Mo2C in aqueous electrolytes in a multimethod experiment and theory approach. We find that surface oxide formation completely suppresses the CO2 activation. The oxides are stable down to potentials as low as −1.9 V versus the standard hydrogen electrode, and solely the hydrogen evolution reaction (HER) is found to be active. This generally points to the absolute imperative of recognizing the true interface establishing under operando conditions in computational screening of catalyst materials. When protected from ambient air and used in nonaqueous electrolyte, Mo2C indeed shows CO2RR activity.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
R W Haid, R M Kluge, T O Schmidt, A S Bandarenka
In-situ Detection of Active Sites for Carbon-Based Bifunctional Oxygen Reduction and Evolution Catalysis Journal Article
In: Electrochimica Acta, vol. 382, pp. 138285, 2021, ISSN: 0013-4686.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {In-situ Detection of Active Sites for Carbon-Based Bifunctional Oxygen Reduction and Evolution Catalysis},
author = {R W Haid and R M Kluge and T O Schmidt and A S Bandarenka},
url = {https://www.sciencedirect.com/science/article/pii/S0013468621005752},
doi = {https://doi.org/10.1016/j.electacta.2021.138285},
issn = {0013-4686},
year = {2021},
date = {2021-04-02},
urldate = {2021-04-02},
journal = {Electrochimica Acta},
volume = {382},
pages = {138285},
abstract = {Due to their availability and electrochemical versatility, carbon-based electrodes are becoming an increasingly popular option as electrocatalysts for fuel cells and metal-air batteries. Additionally, they show great potential as bifunctional catalysts for the oxygen reduction and evolution reaction (ORR/OER) in an alkaline medium. However, to compete with state-of-the-art catalysts, the nature of the active sites and the surface stability under reaction conditions need to be understood in depth. Here, we present a principle study on highly oriented pyrolytic graphite (HOPG), evaluating the surface behavior under both ORR and OER conditions in 0.1 M KOH. We use noise analysis in electrochemical scanning tunneling microscopy (n-EC-STM) to monitor and compare ORR and OER active sites with resolution down to the nanoscale. Furthermore, surface degradation can be evaluated during the operation. We find that close to the respective reaction onset, step sites and defects are active for both ORR and OER. Terraces sites are largely inactive and only become involved in the OER at higher potentials. This could imply corrosion of the carbon. However, since the observed surface structures remain unaltered before and after applying the OER in our experiments, we find no clear evidence of surface destruction. These fundamental insights could inspire further research concerning the active sites and stability of carbon-based catalysts as well as carbon support structures, to discover ways to tune the surface activity and stability to the dedicated purpose.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
H Li, K Liu, J Fu, K Chen, K Yang, Y Lin, B Yang, Q Wang, H Pan, Z Cai, H Li, M Cao, J Hu, Y-R Lu, T-S Chan, E Cortés, A Fratalocchi, M Liu
Paired Ru‒O‒Mo ensemble for efficient and stable alkaline hydrogen evolution reaction Journal Article
In: Nano Energy, vol. 82, pp. 105767, 2021, ISSN: 2211-2855.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Paired Ru‒O‒Mo ensemble for efficient and stable alkaline hydrogen evolution reaction},
author = {H Li and K Liu and J Fu and K Chen and K Yang and Y Lin and B Yang and Q Wang and H Pan and Z Cai and H Li and M Cao and J Hu and Y-R Lu and T-S Chan and E Cort\'{e}s and A Fratalocchi and M Liu},
url = {http://www.sciencedirect.com/science/article/pii/S2211285521000252},
doi = {https://doi.org/10.1016/j.nanoen.2021.105767},
issn = {2211-2855},
year = {2021},
date = {2021-04-01},
urldate = {2021-04-01},
journal = {Nano Energy},
volume = {82},
pages = {105767},
abstract = {Electrocatalytic hydrogen evolution reaction (HER) in alkaline media is a promising electrochemical energy conversion strategy. Ruthenium (Ru) is an efficient catalyst with a desirable cost for HER, however, the sluggish H2O dissociation process, due to the low H2O adsorption on its surface, currently hampers the performances of this catalyst in alkaline HER. Herein, we demonstrate that the H2O adsorption improves significantly by the construction of Ru\textendashO\textendashMo sites. We prepared Ru/MoO2 catalysts with Ru\textendashO\textendashMo sites through a facile thermal treatment process and assessed the creation of Ru\textendashO\textendashMo interfaces by transmission electron microscope (TEM) and extended X-ray absorption fine structure (EXAFS). By using Fourier-transform infrared spectroscopy (FTIR) and H2O adsorption tests, we proved Ru\textendashO\textendashMo sites have tenfold stronger H2O adsorption ability than that of Ru catalyst. The catalysts with Ru\textendashO\textendashMo sites exhibited a state-of-the-art overpotential of 16 mV at 10 mA cm\textendash2 in 1 M KOH electrolyte, demonstrating a threefold reduction than the previous bests of Ru (59 mV) and commercial Pt (31 mV) catalysts. We proved the stability of these performances over 40 h without decline. These results could open a new path for designing efficient and stable catalysts.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
R M Kluge, R W Haid, A S Bandarenka
Assessment of active areas for the oxygen evolution reaction on an amorphous iridium oxide surface Journal Article
In: Journal of Catalysis, vol. 396, pp. 14-22, 2021, ISSN: 0021-9517.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Assessment of active areas for the oxygen evolution reaction on an amorphous iridium oxide surface},
author = {R M Kluge and R W Haid and A S Bandarenka},
url = {https://www.sciencedirect.com/science/article/pii/S0021951721000531},
doi = {https://doi.org/10.1016/j.jcat.2021.02.007},
issn = {0021-9517},
year = {2021},
date = {2021-04-01},
urldate = {2021-04-01},
journal = {Journal of Catalysis},
volume = {396},
pages = {14-22},
abstract = {Electrocatalytic “green” production of hydrogen from water for sustainable energy provision schemes is currently inefficient due to the sluggish kinetics of the oxygen evolution reaction (OER) at the anodes of the electrolysers. In the case of acidic polymer electrolyte membrane electrolysers, iridium (Ir) oxide catalysts pose a promising compromise between good OER activity and stability. However, the structure\textendashactivity relations for these materials remain largely unknown because the surface of a “real” oxide catalyst under reaction conditions becomes amorphous. In order to contribute to the understanding of these systems, we use electrochemical scanning tunnelling microscopy under reaction conditions (‘noise’ or n-EC-STM). With this technique, active areas can be detected by an increased noise level of the STM signal compared to inactive sites. The n-EC-STM measurements are applied to an amorphous iridium oxide surface, which is formed during electrochemical cycling of Ir(111). By doing so, we can monitor OER activity in-situ while simultaneously assessing the surface morphology. In order to elucidate the active areas, step and terrace sites were quantitatively compared to each other. The measurements reveal that terraces, step sites and concavities lead to a similar noise level increase in the STM signal. We, thus, conclude that the OER on the amorphous extended iridium oxide surface shows little structure-sensitivity. Subsequently, we suggest that in contrast to, e.g., metallic Pt for the oxygen electro-reduction, the shape of amorphous IrOx nanoparticles in an acidic medium should not significantly influence the OER turnover frequency.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
R Kluge, R W Haid, I Stephens, F Calle-Vallejo, A S Bandarenka
Monitoring Active Sites for Hydrogen Evolution Reaction at Model Carbon Surfaces Journal Article
In: Physical Chemistry Chemical Physics, vol. 23, pp. 10051-10058, 2021, ISSN: 1463-9076.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Monitoring Active Sites for Hydrogen Evolution Reaction at Model Carbon Surfaces},
author = {R Kluge and R W Haid and I Stephens and F Calle-Vallejo and A S Bandarenka},
url = {http://dx.doi.org/10.1039/D1CP00434D},
doi = {10.1039/D1CP00434D},
issn = {1463-9076},
year = {2021},
date = {2021-03-25},
urldate = {2021-03-25},
journal = {Physical Chemistry Chemical Physics},
volume = {23},
pages = {10051-10058},
abstract = {Carbon is ubiquitous as an electrode material in electrochemical energy conversion devices. If used as support material, the evolution of H2 is undesired on carbon. However, recently carbon-based materials are of high interest as economic and eco-conscious alternative to noble metal catalysts. The targeted design of improved carbon electrode materials requires atomic scale insight into the structure of the sites that catalyse H2 evolution. This work demonstrates that electrochemical scanning tunnelling microscopy under reaction conditions (n-EC-STM) can monitor active sites of highly oriented pyrolytic graphite for the hydrogen evolution reaction. With down to atomic resolution, the most active sites in acidic medium are pinpointed near edge sites and defects, whereas the basal planes remain inactive. Density functional theory calculations support these findings and reveal that only specific defects on graphite are active. Motivated by these results, the extensive usage of n-EC-STM on doped carbon-based materials is encouraged to locate their active sites and guide the synthesis of enhanced electrocatalysts.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
A Auer, X Ding, A S Bandarenka, J Kunze-Liebhäuser
The Potential of Zero Charge and the Electrochemical Interface Structure of Cu(111) in Alkaline Solutions Journal Article
In: The Journal of Physical Chemistry C, vol. 125, pp. 5020-5028, 2021, ISSN: 1932-7447.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {The Potential of Zero Charge and the Electrochemical Interface Structure of Cu(111) in Alkaline Solutions},
author = {A Auer and X Ding and A S Bandarenka and J Kunze-Liebh\"{a}user},
url = {https://doi.org/10.1021/acs.jpcc.0c09289},
doi = {10.1021/acs.jpcc.0c09289},
issn = {1932-7447},
year = {2021},
date = {2021-03-01},
urldate = {2021-03-01},
journal = {The Journal of Physical Chemistry C},
volume = {125},
pages = {5020-5028},
abstract = {Copper (Cu) is a unique electrocatalyst, which is able to efficiently oxidize CO at very low overpotentials and reduce CO2 to valuable fuels with reasonable Faradaic efficiencies. Yet, knowledge of its electrochemical properties at the solid/liquid interface is still scarce. Here, we present the first two-stranded correlation of the potential of zero free charge (pzfc) of Cu(111) in alkaline electrolyte at different pH values through application of nanosecond laser pulses and the corresponding interfacial structure changes by in situ electrochemical scanning tunneling microscopy imaging. The pzfc of Cu(111) at pH 13 is identified at −0.73 VSHE in the apparent double layer region, prior to the onset of hydroxide adsorption. It shifts by (88 ± 4) mV to more positive potentials per decreasing pH unit. At the pzfc, Cu(111) shows structural dynamics at both pH 13 and pH 11, which can be understood as the onset of surface restructuring. At higher potentials, full reconstruction and electric field dependent OH adsorption occurs, which causes a remarkable decrease in the atomic density of the first Cu layer. The expansion of the Cu\textendashCu distance to 0.3 nm generates a hexagonal Moir\'{e} pattern, on which the adsorbed OH forms a commensurate (1 × 2) adlayer structure with a steady state coverage of 0.5 monolayers at pH 13. Our experimental findings shed light on the true charge distribution and its interrelation with the atomic structure of the electrochemical interface of Cu.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
M Wörle, A W Holleitner, R Kienberger, H Iglev
Ultrafast hot carrier relaxation in silicon monitored by phase-resolved transient absorption spectroscopy Journal Article
In: arXiv preprint arXiv:2101.01439, 2021.
Tags: Solid-Liquid
@article{,
title = {Ultrafast hot carrier relaxation in silicon monitored by phase-resolved transient absorption spectroscopy},
author = {M W\"{o}rle and A W Holleitner and R Kienberger and H Iglev},
year = {2021},
date = {2021-01-05},
journal = {arXiv preprint arXiv:2101.01439},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
P H C Camargo, E Cortés
Plasmonic Catalysis: From Fundamentals to Applications Book
Wiley, 2021, ISBN: 9783527347506.
Links | Tags: Foundry Inorganic, Solid-Liquid, Solid-Solid
@book{,
title = {Plasmonic Catalysis: From Fundamentals to Applications},
author = {P H C Camargo and E Cort\'{e}s},
url = {https://books.google.de/books?id=jMEqEAAAQBAJ},
isbn = {9783527347506},
year = {2021},
date = {2021-01-01},
publisher = {Wiley},
keywords = {Foundry Inorganic, Solid-Liquid, Solid-Solid},
pubstate = {published},
tppubtype = {book}
}
J B Lee, H Walker, Y Li, T W Nam, A Rakovich, R Sapienza, Y S Jung, Y S Nam, S A Maier, E Cortés
Template Dissolution Interfacial Patterning of Single Colloids for Nanoelectrochemistry and Nanosensing Journal Article
In: ACS Nano, 2020, ISSN: 1936-0851.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Template Dissolution Interfacial Patterning of Single Colloids for Nanoelectrochemistry and Nanosensing},
author = {J B Lee and H Walker and Y Li and T W Nam and A Rakovich and R Sapienza and Y S Jung and Y S Nam and S A Maier and E Cort\'{e}s},
url = {https://doi.org/10.1021/acsnano.0c09319},
doi = {10.1021/acsnano.0c09319},
issn = {1936-0851},
year = {2020},
date = {2020-12-03},
urldate = {2020-12-03},
journal = {ACS Nano},
abstract = {Deterministic positioning and assembly of colloidal nanoparticles (NPs) onto substrates is a core requirement and a promising alternative to top-down lithography to create functional nanostructures and nanodevices with intriguing optical, electrical, and catalytic features. Capillary-assisted particle assembly (CAPA) has emerged as an attractive technique to this end, as it allows controlled and selective assembly of a wide variety of NPs onto predefined topographical templates using capillary forces. One critical issue with CAPA, however, lies in its final printing step, where high printing yields are possible only with the use of an adhesive polymer film. To address this problem, we have developed a template dissolution interfacial patterning (TDIP) technique to assemble and print single colloidal AuNP arrays onto various dielectric and conductive substrates in the absence of any adhesion layer, with printing yields higher than 98%. The TDIP approach grants direct access to the interface between the AuNP and the target surface, enabling the use of colloidal AuNPs as building blocks for practical applications. The versatile applicability of TDIP is demonstrated by the creation of direct electrical junctions for electro- and photoelectrochemistry and nanoparticle-on-mirror geometries for single-particle molecular sensing.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
L Wolz, C Heshmatpour, A Perri, D Polli, G Cerullo, J J Finley, E Thyrhaug, J Hauer, A V Stier
Time-domain photocurrent spectroscopy based on a common-path birefringent interferometer Journal Article
In: Review of Scientific Instruments, vol. 91, no. 12, pp. 123101, 2020.
Links | Tags: Solid-Liquid
@article{,
title = {Time-domain photocurrent spectroscopy based on a common-path birefringent interferometer},
author = {L Wolz and C Heshmatpour and A Perri and D Polli and G Cerullo and J J Finley and E Thyrhaug and J Hauer and A V Stier},
url = {https://aip.scitation.org/doi/abs/10.1063/5.0023543},
doi = {10.1063/5.0023543},
year = {2020},
date = {2020-12-02},
urldate = {2020-12-02},
journal = {Review of Scientific Instruments},
volume = {91},
number = {12},
pages = {123101},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
S Pratap, J Schlipf, L Bießmann, P Müller-Buschbaum
Hierarchical Structures from Nanocrystalline Colloidal Precursors within Hybrid Perovskite Thin Films: Implications for Photovoltaics Journal Article
In: ACS Applied Nano Materials, vol. 3, no. 12, pp. 11701-11708, 2020.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Hierarchical Structures from Nanocrystalline Colloidal Precursors within Hybrid Perovskite Thin Films: Implications for Photovoltaics},
author = {S Pratap and J Schlipf and L Bie\ssmann and P M\"{u}ller-Buschbaum},
url = {https://doi.org/10.1021/acsanm.0c03000},
doi = {10.1021/acsanm.0c03000},
year = {2020},
date = {2020-11-23},
urldate = {2020-11-23},
journal = {ACS Applied Nano Materials},
volume = {3},
number = {12},
pages = {11701-11708},
abstract = {Originating from stochastic nanocrystalline colloidal precursors with differential chemical compositions, crystalline thin films exhibit hierarchical structures originating at the crystallographic level and scaling up to mesoscale structures, manifested within their nanocrystalline morphology and mesoscale topology. We interlink morphogenetic signatures within thin films to differential precursor chemistry and explain the cooperative impact of structure-defining inorganic and organic counterparts on perovskite hybrids. Understanding the effect of chemical species on the structural characteristics of thin films and leveraging complex assembly processes present facile routes to tuning multiscale morphologies in thin films, pertinent for engineering functional performance metrics within thin-film perovskite photovoltaics.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
D Böhm, M Beetz, C Kutz, S Zhang, C Scheu, T Bein, D Fattakhova-Rohlfing
In: Chemistry of Materials, vol. 32, no. 24, pp. 10394-10406, 2020, ISSN: 0897-4756.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {V(III)-Doped Nickel Oxide-Based Nanocatalysts for Electrochemical Water Splitting: Influence of Phase, Composition, and Doping on the Electrocatalytic Activity},
author = {D B\"{o}hm and M Beetz and C Kutz and S Zhang and C Scheu and T Bein and D Fattakhova-Rohlfing},
url = {https://doi.org/10.1021/acs.chemmater.0c02851},
doi = {10.1021/acs.chemmater.0c02851},
issn = {0897-4756},
year = {2020},
date = {2020-11-16},
journal = {Chemistry of Materials},
volume = {32},
number = {24},
pages = {10394-10406},
abstract = {Doped nickel oxide-based compounds are attracting great interest as very efficient and abundant catalysts and were thoroughly investigated as battery materials in the past. However, there is still no clear understanding of the influence of dopants on the complex dynamic character of their chemically and potentially driven transformations. We have developed a synthesis procedure enabling the controlled formation of nanosized nickel hydroxide and nickel oxide polymorphs substituted with vanadium(III) [V(III)] ions and further investigated their structure\textendashactivity correlation for electrochemical water oxidation. This work therefore primarily focuses on an in-depth structural characterization of the homogeneously doped nanosized α- and β-Ni(OH)2 polymorphs. It could be shown that concentrations of 10 at. % V(III) and higher can effectively inhibit a spontaneous phase transformation known as chemical aging of the turbostratic α-phase to the more crystalline β-Ni(OH)2 phase in neutral aqueous media. The Fe-impurity-biased electrocatalytic activity determined for α-/β-Ni1\textendashxVx(OH)2 showed only a minor increase of 10% oxygen evolution reaction (OER) activity for an 1 at. % doped nonaged sample resembling the α-phase, while a 5 at. % V(III)-doped sample chemically aged over 24 h led to a doubled OER activity versus the undoped reference which transformed into β-Ni(OH)2 over that period of time.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
Y Xiao, C Feng, J Fu, F Wang, C Li, V F Kunzelmann, C-M Jiang, M Nakabayashi, N Shibata, I D Sharp, K Domen, Y Li
Band structure engineering and defect control of Ta3N5 for efficient photoelectrochemical water oxidation Journal Article
In: Nature Catalysis, vol. 3, no. 11, pp. 932-940, 2020, ISSN: 2520-1158.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Band structure engineering and defect control of Ta3N5 for efficient photoelectrochemical water oxidation},
author = {Y Xiao and C Feng and J Fu and F Wang and C Li and V F Kunzelmann and C-M Jiang and M Nakabayashi and N Shibata and I D Sharp and K Domen and Y Li},
url = {https://doi.org/10.1038/s41929-020-00522-9},
doi = {10.1038/s41929-020-00522-9},
issn = {2520-1158},
year = {2020},
date = {2020-11-01},
urldate = {2020-11-01},
journal = {Nature Catalysis},
volume = {3},
number = {11},
pages = {932-940},
abstract = {Ta3N5 is a promising photoanode material with a theoretical maximum solar conversion efficiency of 15.9% for photoelectrochemical water splitting. However, the highest applied bias photon-to-current efficiency achieved so far is only 2.72%. To bridge the efficiency gap, effective carrier management strategies for Ta3N5 photoanodes should be developed. Here, we propose to use gradient Mg doping for band structure engineering and defect control of Ta3N5. The gradient Mg doping profile in Ta3N5 induces a gradient of the band edge energetics, which greatly enhances the charge separation efficiency. Furthermore, defect-related recombination is significantly suppressed due to the passivation effect of Mg dopants on deep-level defects and, more importantly, the matching of the gradient Mg doping profile with the distribution of defects within Ta3N5. As a result, a photoanode based on the gradient Mg-doped Ta3N5 delivers a low onset potential of 0.4 V versus that of a reversible hydrogen electrode and a high applied bias photon-to-current efficiency of 3.25 ± 0.05%.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
A Mähringer, M Hennemann, T Clark, T Bein, D D Medina
Energy Efficient Ultrahigh Flux Separation of Oily Pollutants from Water with Superhydrophilic Nanoscale Metal–Organic Framework Architectures Journal Article
In: Angewandte Chemie International Edition, vol. 60, no. 10, pp. 5519-5526, 2020, ISSN: 1433-7851.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{nokey,
title = {Energy Efficient Ultrahigh Flux Separation of Oily Pollutants from Water with Superhydrophilic Nanoscale Metal\textendashOrganic Framework Architectures},
author = {A M\"{a}hringer and M Hennemann and T Clark and T Bein and D D Medina},
url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202012428},
doi = {https://doi.org/10.1002/anie.202012428},
issn = {1433-7851},
year = {2020},
date = {2020-10-05},
journal = {Angewandte Chemie International Edition},
volume = {60},
number = {10},
pages = {5519-5526},
abstract = {Abstract The rising demand for clean water for a growing and increasingly urban global population is one of the most urgent issues of our time. Here, we introduce the synthesis of a unique nanoscale architecture of pillar-like Co-CAT-1 metal\textendashorganic framework (MOF) crystallites on gold-coated woven stainless steel meshes with large, 50 μm apertures. These nanostructured mesh surfaces feature superhydrophilic and underwater superoleophobic wetting properties, allowing for gravity-driven, highly efficient oil\textendashwater separation featuring water fluxes of up to nearly one million L m−2 h−1. Water physisorption experiments reveal the hydrophilic nature of Co-CAT-1 with a total water vapor uptake at room temperature of 470 cm3 g−1. Semiempirical molecular orbital calculations shed light on water affinity of the inner and outer pore surfaces. The MOF-based membranes enable high separation efficiencies for a number of liquids tested, including the notorious water pollutant, crude oil, affording chemical oxygen demand (COD) concentrations below 25 mg L−1 of the effluent. Our results demonstrate the great impact of suitable nanoscale surface architectures as a means of encoding on-surface extreme wetting properties, yielding energy-efficient water-selective large-aperture membranes.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
Del F Giudice, J Becker, De C Rose, M Döblinger, D Ruhstorfer, L Suomenniemi, J Treu, H Riedl, J J Finley, G Koblmüller
Ultrathin catalyst-free InAs nanowires on silicon with distinct 1D sub-band transport properties Journal Article
In: Nanoscale, vol. 12, no. 42, pp. 21857-21868, 2020, ISSN: 2040-3364.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Ultrathin catalyst-free InAs nanowires on silicon with distinct 1D sub-band transport properties},
author = {Del F Giudice and J Becker and De C Rose and M D\"{o}blinger and D Ruhstorfer and L Suomenniemi and J Treu and H Riedl and J J Finley and G Koblm\"{u}ller},
url = {http://dx.doi.org/10.1039/D0NR05666A},
doi = {10.1039/D0NR05666A},
issn = {2040-3364},
year = {2020},
date = {2020-10-01},
journal = {Nanoscale},
volume = {12},
number = {42},
pages = {21857-21868},
abstract = {Ultrathin InAs nanowires (NW) with a one-dimensional (1D) sub-band structure are promising materials for advanced quantum-electronic devices, where dimensions in the sub-30 nm diameter limit together with post-CMOS integration scenarios on Si are much desired. Here, we demonstrate two site-selective synthesis methods that achieve epitaxial, high aspect ratio InAs NWs on Si with ultrathin diameters below 20 nm. The first approach exploits direct vapor\textendashsolid growth to tune the NW diameter by interwire spacing, mask opening size and growth time. The second scheme explores a unique reverse-reaction growth by which the sidewalls of InAs NWs are thermally decomposed under controlled arsenic flux and annealing time. Interesting kinetically limited dependencies between interwire spacing and thinning dynamics are found, yielding diameters as low as 12 nm for sparse NW arrays. We clearly verify the 1D sub-band structure in ultrathin NWs by pronounced conductance steps in low-temperature transport measurements using back-gated NW-field effect transistors. Correlated simulations reveal single- and double degenerate conductance steps, which highlight the rotational hexagonal symmetry and reproduce the experimental traces in the diffusive 1D transport limit. Modelling under the realistic back-gate configuration further evidences regimes that lead to asymmetric carrier distribution and breakdown of the degeneracy depending on the gate bias.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
J Fu, F Wang, Y Xiao, Y Yao, C Feng, L Chang, C-M Jiang, V F Kunzelmann, Z M Wang, A O Govorov, I D Sharp, Y Li
Identifying Performance-Limiting Deep Traps in Ta3N5 for Solar Water Splitting Journal Article
In: ACS Catalysis, vol. 10, no. 18, pp. 10316-10324, 2020.
Abstract | Links | Tags: Solid-Liquid
@article{,
title = {Identifying Performance-Limiting Deep Traps in Ta3N5 for Solar Water Splitting},
author = {J Fu and F Wang and Y Xiao and Y Yao and C Feng and L Chang and C-M Jiang and V F Kunzelmann and Z M Wang and A O Govorov and I D Sharp and Y Li},
url = {https://doi.org/10.1021/acscatal.0c02648},
doi = {10.1021/acscatal.0c02648},
year = {2020},
date = {2020-09-18},
journal = {ACS Catalysis},
volume = {10},
number = {18},
pages = {10316-10324},
abstract = {Ta3N5 is a promising semiconductor for solar-driven photocatalytic or photoelectrochemical (PEC) water splitting. However, the lack of an in-depth understanding of its intrinsic defect properties limits further improvement of its performance. In this study, comprehensive spectroscopic characterizations are combined with theoretical calculations to investigate the defect properties of Ta3N5. The obtained electronic structure of Ta3N5 reveals that oxygen impurities are shallow donors, while nitrogen vacancies and reduced Ta centers (Ta3+) are deep traps. The Ta3+ defects are identified to be most detrimental to the water splitting performance because their energetic position lies below the water reduction potential. Based on these findings, a simple H2O2 pretreatment method is employed to improve the PEC performance of the Ta3N5 photoanode by reducing the concentration of Ta3+ defects, resulting in a high solar-to-hydrogen conversion efficiency of 2.25%. The fundamental knowledge about the defect properties of Ta3N5 could serve as a guideline for developing more efficient photoanodes and photocatalysts.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
S Morozov, E L Pensa, A H Khan, A Polovitsyn, E Cortés, S A Maier, S Vezzoli, I Moreels, R Sapienza
Electrical control of single-photon emission in highly charged individual colloidal quantum dots Journal Article
In: Sci Adv, vol. 6, no. 38, 2020, ISSN: 2375-2548.
Abstract | Links | Tags: Solid-Liquid, Solid-Solid
@article{nokey,
title = {Electrical control of single-photon emission in highly charged individual colloidal quantum dots},
author = {S Morozov and E L Pensa and A H Khan and A Polovitsyn and E Cort\'{e}s and S A Maier and S Vezzoli and I Moreels and R Sapienza},
url = {https://pubmed.ncbi.nlm.nih.gov/32948584/},
doi = {10.1126/sciadv.abb1821},
issn = {2375-2548},
year = {2020},
date = {2020-09-18},
urldate = {2020-09-18},
journal = {Sci Adv},
volume = {6},
number = {38},
abstract = {Electron transfer to an individual quantum dot promotes the formation of charged excitons with enhanced recombination pathways and reduced lifetimes. Excitons with only one or two extra charges have been observed and exploited for very efficient lasing or single-quantum dot light-emitting diodes. Here, by room-temperature time-resolved experiments on individual giant-shell CdSe/CdS quantum dots, we show the electrochemical formation of highly charged excitons containing more than 12 electrons and 1 hole. We report the control over intensity blinking, along with a deterministic manipulation of quantum dot photodynamics, with an observed 210-fold increase in the decay rate, accompanied by 12-fold decrease in the emission intensity, while preserving single-photon emission characteristics. These results pave the way for deterministic control over the charge state, and room-temperature decay rate engineering for colloidal quantum dot-based classical and quantum communication technologies.},
keywords = {Solid-Liquid, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
W Kaiser, A Gagliardi
In: Entropy, vol. 22, no. 9, pp. 1013, 2020, ISSN: 1099-4300.
Abstract | Links | Tags: Solid-Liquid, Solid-Solid
@article{nokey,
title = {Stepping Out of Equilibrium: The Quest for Understanding the Role of Non-Equilibrium (Thermo-)Dynamics in Electronic and Electrochemical Processes},
author = {W Kaiser and A Gagliardi},
url = {https://www.mdpi.com/1099-4300/22/9/1013},
issn = {1099-4300},
year = {2020},
date = {2020-09-10},
journal = {Entropy},
volume = {22},
number = {9},
pages = {1013},
abstract = {This editorial aims to interest researchers and inspire novel research on the topic of non-equilibrium Thermodynamics and Monte Carlo for Electronic and Electrochemical Processes. We present a brief outline on recent progress and challenges in the study of non-equilibrium dynamics and thermodynamics using numerical Monte Carlo simulations. The aim of this special issue is to collect recent advances and novel techniques of Monte Carlo methods to study non-equilibrium electronic and electrochemical processes at the nanoscale.},
keywords = {Solid-Liquid, Solid-Solid},
pubstate = {published},
tppubtype = {article}
}
N G Hörmann, N Marzari, K Reuter
Electrosorption at metal surfaces from first principles Journal Article
In: npj Computational Materials, vol. 6, no. 1, pp. 136, 2020, ISSN: 2057-3960.
Abstract | Links | Tags: Solid-Liquid
@article{nokey,
title = {Electrosorption at metal surfaces from first principles},
author = {N G H\"{o}rmann and N Marzari and K Reuter},
url = {https://doi.org/10.1038/s41524-020-00394-4},
doi = {10.1038/s41524-020-00394-4},
issn = {2057-3960},
year = {2020},
date = {2020-09-08},
urldate = {2020-09-08},
journal = {npj Computational Materials},
volume = {6},
number = {1},
pages = {136},
abstract = {Electrosorption of solvated species at metal electrodes is a most fundamental class of processes in interfacial electrochemistry. Here, we use its sensitive dependence on the electric double layer to assess the performance of ab initio thermodynamics approaches increasingly used for the first-principles description of electrocatalysis. We show analytically that computational hydrogen electrode calculations at zero net-charge can be understood as a first-order approximation to a fully grand canonical approach. Notably, higher-order terms in the applied potential caused by the charging of the double layer include contributions from adsorbate-induced changes in the work function and in the interfacial capacitance. These contributions are essential to yield prominent electrochemical phenomena such as non-Nernstian shifts of electrosorption peaks and non-integer electrosorption valencies. We illustrate this by calculating peak shifts for H on Pt electrodes and electrosorption valencies of halide ions on Ag electrodes, obtaining qualitative agreement with experimental data already when considering only second order terms. The results demonstrate the agreement between classical electrochemistry concepts and a first-principles fully grand canonical description of electrified interfaces and shed new light on the widespread computational hydrogen electrode approach.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
A Auer, M Andersen, E-M Wernig, N G Hörmann, N Buller, K Reuter, J Kunze-Liebhäuser
Self-activation of copper electrodes during CO electro-oxidation in alkaline electrolyte Journal Article
In: Nature Catalysis, 2020, ISSN: 2520-1158.
Abstract | Links | Tags: Solid-Liquid
@article{,
title = {Self-activation of copper electrodes during CO electro-oxidation in alkaline electrolyte},
author = {A Auer and M Andersen and E-M Wernig and N G H\"{o}rmann and N Buller and K Reuter and J Kunze-Liebh\"{a}user},
url = {https://doi.org/10.1038/s41929-020-00505-w},
doi = {10.1038/s41929-020-00505-w},
issn = {2520-1158},
year = {2020},
date = {2020-09-07},
journal = {Nature Catalysis},
abstract = {The development of low-temperature fuel cells for clean energy production is an appealing alternative to fossil-fuel technologies. CO is a key intermediate in the electro-oxidation of energy carrying fuels and, due to its strong interaction with state-of-the-art Pt electrodes, it is known to act as a poison. Here we demonstrate the ability of Earth-abundant Cu to electro-oxidize CO efficiently in alkaline media, reaching high current densities of ≥0.35 mA cm−2 on single-crystal Cu(111) model catalysts. Strong and continuous surface structural changes are observed under reaction conditions. Supported by first-principles microkinetic modelling, we show that the concomitant presence of high-energy undercoordinated Cu structures at the surface is a prerequisite for the high activity. Similar CO-induced self-activation has been reported for gas\textendashsurface reactions at coinage metals, demonstrating the strong parallels between heterogeneous thermal catalysis and heterogeneous electrocatalysis.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
L D M Peters, J Kussmann, C Ochsenfeld
In: The Journal of Chemical Physics, vol. 153, no. 9, pp. 094104, 2020.
Abstract | Links | Tags: Molecularly-Functionalized, Solid-Liquid
@article{nokey,
title = {A Fermi smearing variant of the Tamm\textendashDancoff approximation for nonadiabatic dynamics involving S1\textendashS0 transitions: Validation and application to azobenzene},
author = {L D M Peters and J Kussmann and C Ochsenfeld},
url = {https://aip.scitation.org/doi/abs/10.1063/5.0016487},
doi = {10.1063/5.0016487},
year = {2020},
date = {2020-09-02},
journal = {The Journal of Chemical Physics},
volume = {153},
number = {9},
pages = {094104},
abstract = {The main shortcoming of time-dependent density functional theory (TDDFT) regarding its use for nonadiabatic molecular dynamics (NAMD) is its incapability to describe conical intersections involving the ground state. To overcome this problem, we combine Fermi smearing (FS) DFT with a fractional-occupation variant of the Tamm\textendashDancoff approximation (TDA) of TDDFT in the generalized gradient approximation. The resulting method (which we denote as FS-TDA) gives access to ground- and excited-state energies, gradients, and nonadiabatic coupling vectors, which are physically correct even in the vicinity of S1\textendashS0 conical intersections. This is shown for azobenzene, a widely used photoswitch, via single point calculations and NAMD simulations of its cis\textendashtrans photoisomerization. We conclude that FS-TDA may be used as an efficient alternative to investigate these processes.},
keywords = {Molecularly-Functionalized, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
G Grinblat, H Zhang, M P Nielsen, L Krivitsky, R Berté, Y Li, B Tilmann, E Cortés, R F Oulton, A I Kuznetsov, S A Maier
Efficient ultrafast all-optical modulation in a nonlinear crystalline gallium phosphide nanodisk at the anapole excitation Journal Article
In: Science Advances, vol. 6, no. 34, pp. eabb3123, 2020.
Abstract | Links | Tags: Solid-Liquid
@article{,
title = {Efficient ultrafast all-optical modulation in a nonlinear crystalline gallium phosphide nanodisk at the anapole excitation},
author = {G Grinblat and H Zhang and M P Nielsen and L Krivitsky and R Bert\'{e} and Y Li and B Tilmann and E Cort\'{e}s and R F Oulton and A I Kuznetsov and S A Maier},
url = {https://advances.sciencemag.org/content/advances/6/34/eabb3123.full.pdf},
doi = {10.1126/sciadv.abb3123},
year = {2020},
date = {2020-08-21},
journal = {Science Advances},
volume = {6},
number = {34},
pages = {eabb3123},
abstract = {High\textendashrefractive index nanostructured dielectrics have the ability to locally enhance electromagnetic fields with low losses while presenting high third-order nonlinearities. In this work, we exploit these characteristics to achieve efficient ultrafast all-optical modulation in a crystalline gallium phosphide (GaP) nanoantenna through the optical Kerr effect (OKE) and two-photon absorption (TPA) in the visible/near-infrared range. We show that an individual GaP nanodisk can yield differential reflectivity modulations of up to ~40%, with characteristic modulation times between 14 and 66 fs, when probed at the anapole excitation (AE). Numerical simulations reveal that the AE represents a unique condition where both the OKE and TPA contribute with the same modulation sign, maximizing the response. These findings highly outperform previous reports on sub\textendash100-fs all-optical switching from resonant nanoscale dielectrics, which have demonstrated modulation depths no larger than 0.5%, placing GaP nanoantennas as a promising choice for ultrafast all-optical modulation at the nanometer scale.},
keywords = {Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}
H A Vignolo-González, S Laha, A Jiménez-Solano, T Oshima, V Duppel, P Schützendübe, B V Lotsch
Toward Standardized Photocatalytic Oxygen Evolution Rates Using RuO2@TiO2 as a Benchmark Journal Article
In: Matter, vol. 3, no. 2, pp. 464-486, 2020, ISSN: 2590-2385.
Abstract | Links | Tags: Foundry Inorganic, Solid-Liquid
@article{,
title = {Toward Standardized Photocatalytic Oxygen Evolution Rates Using RuO2@TiO2 as a Benchmark},
author = {H A Vignolo-Gonz\'{a}lez and S Laha and A Jim\'{e}nez-Solano and T Oshima and V Duppel and P Sch\"{u}tzend\"{u}be and B V Lotsch},
url = {http://www.sciencedirect.com/science/article/pii/S2590238520303799},
doi = {https://doi.org/10.1016/j.matt.2020.07.021},
issn = {2590-2385},
year = {2020},
date = {2020-08-05},
journal = {Matter},
volume = {3},
number = {2},
pages = {464-486},
abstract = {Summary Quantitative comparison of photocatalytic performances across different photocatalysis setups is technically challenging. Here, we combine the concepts of relative and optimal photonic efficiencies to normalize activities with an internal benchmark material, RuO2 photodeposited on a P25-TiO2 photocatalyst, which was optimized for reproducibility of the oxygen evolution reaction (OER). Additionally, a general set of good practices was identified to ensure reliable quantification of photocatalytic OER, including photoreactor design, photocatalyst dispersion, and control of parasitic reactions caused by the sacrificial electron acceptor. Moreover, a method combining optical modeling and measurements was proposed to quantify the benchmark absorbed and scattered light (7.6% and 81.2%, respectively, of λ = 300\textendash500 nm incident photons), rather than just incident light (≈AM 1.5G), to estimate its internal quantum efficiency (16%). We advocate the adoption of the instrumental and theoretical framework provided here to facilitate material standardization and comparison in the field of artificial photosynthesis.},
keywords = {Foundry Inorganic, Solid-Liquid},
pubstate = {published},
tppubtype = {article}
}