Prof. Dr. Jennifer Rupp
Academic Research Focus
- Solid state materials for sustainable energy storage and conversion
- Solid state batteries
- Redox flow batteries
- Solid oxide fuel cells
- Solid state batteries
- Redox flow batteries
- Solid oxide fuel cells
Fields of Application
Batteries, Fuel Cells, Semiconductor Materials, Solar Fuels
Publications
12.
H Y W Chu, C Lerch, S G Y Chong, L Schulz, T Fuchs, K J Kim, M Balaish, H L Tuller, J Janek, J L M Rupp
Solubility-guided interlayer design toward balanced lithium metal plating and stripping in garnet solid-state batteries Journal Article
In: Energy & Environmental Science, vol. 19, no. 17, pp. 5836-5856, 2026, ISSN: 1754-5692.
@article{nokey,
title = {Solubility-guided interlayer design toward balanced lithium metal plating and stripping in garnet solid-state batteries},
author = {H Y W Chu and C Lerch and S G Y Chong and L Schulz and T Fuchs and K J Kim and M Balaish and H L Tuller and J Janek and J L M Rupp},
url = {\<Go to ISI\>://WOS:001850501800001},
doi = {10.1039/d6ee03852b},
issn = {1754-5692},
year = {2026},
date = {2026-09-01},
journal = {Energy \& Environmental Science},
volume = {19},
number = {17},
pages = {5836-5856},
abstract = {The metal-electrolyte interface poses a major challenge in solid-state lithium-metal batteries due to interfacial delamination and dendrite penetration. Although lithium-alloying metal interlayers have been studied to stabilize the interface, a unified framework to compare their relative effectiveness remains limited. This study proposes a lithiophilicity-guided strategy to select optimal anode interlayers for Li-garnet electrolytes, assessing lithiophilicity via lithium solubility in the host metal. Copper, gold, and silver were chosen to represent low, intermediate, and high lithiophilicity, respectively, based on their binary phase diagrams. During cycling, copper's low lithiophilicity led to limited lithium nucleation and uneven growth, whereas silver's high lithiophilicity enabled controlled plating but caused vacancy formation and void aggregation upon stripping. Gold, with intermediate lithiophilicity, achieved balanced performance by supporting uniform plating and stripping at current densities above 1 mA cm-2. Building on the correlation, platinum was identified as a promising candidate with moderate lithium solubility, achieving low interfacial resistance (1 Omega cm2) and a high critical current density (1.2 mA cm-2). Lithiophilicity, a thermodynamically accessible and empirically grounded descriptor, serves as a reliable criterion for metallic interlayer material selection. This guideline can accelerate the discovery of high-performance interlayers and the development of stable solid-solid interfaces in next-generation lithium batteries.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The metal-electrolyte interface poses a major challenge in solid-state lithium-metal batteries due to interfacial delamination and dendrite penetration. Although lithium-alloying metal interlayers have been studied to stabilize the interface, a unified framework to compare their relative effectiveness remains limited. This study proposes a lithiophilicity-guided strategy to select optimal anode interlayers for Li-garnet electrolytes, assessing lithiophilicity via lithium solubility in the host metal. Copper, gold, and silver were chosen to represent low, intermediate, and high lithiophilicity, respectively, based on their binary phase diagrams. During cycling, copper's low lithiophilicity led to limited lithium nucleation and uneven growth, whereas silver's high lithiophilicity enabled controlled plating but caused vacancy formation and void aggregation upon stripping. Gold, with intermediate lithiophilicity, achieved balanced performance by supporting uniform plating and stripping at current densities above 1 mA cm-2. Building on the correlation, platinum was identified as a promising candidate with moderate lithium solubility, achieving low interfacial resistance (1 Omega cm2) and a high critical current density (1.2 mA cm-2). Lithiophilicity, a thermodynamically accessible and empirically grounded descriptor, serves as a reliable criterion for metallic interlayer material selection. This guideline can accelerate the discovery of high-performance interlayers and the development of stable solid-solid interfaces in next-generation lithium batteries.
11.
R B Church, M T Robinson, S C Sand, L P Kong, J L M Rupp, A J Hart
A Proof-of-Concept Interdigitated 3D Lithium-Ion Battery Cell Architecture Using Patterned Carbon Nanotube Forests Journal Article
In: Journal of the Electrochemical Society, vol. 173, no. 16, 2026, ISSN: 0013-4651.
@article{nokey,
title = {A Proof-of-Concept Interdigitated 3D Lithium-Ion Battery Cell Architecture Using Patterned Carbon Nanotube Forests},
author = {R B Church and M T Robinson and S C Sand and L P Kong and J L M Rupp and A J Hart},
url = {\<Go to ISI\>://WOS:001861249100001},
doi = {10.1149/1945-7111/ae81f3},
issn = {0013-4651},
year = {2026},
date = {2026-08-28},
journal = {Journal of the Electrochemical Society},
volume = {173},
number = {16},
abstract = {Planar lithium-ion cells with thick electrodes are often subject to an inherent tradeoff between energy and power density due to tortuous lithium-ion diffusion distances through the porous electrodes. Interdigitated 3D cell architectures circumvent this problem by incorporating thick electrode designs while also keeping lithium-ion diffusion distances short, thereby enabling cells with high energy and power densities. However, attempts to fabricate interdigitated cells have been hindered by difficulty in producing conformally coated electrolytes and incorporating the second electrode. Previously, we demonstrated that patterned vertically aligned carbon nanotubes (VA-CNTs) grown directly on Cu foil and coated with Si thin films could serve as a versatile template for high energy density 3D electrodes. Here, we investigate these Si-CNT composites as a template for 3D full cell design. Initiated chemical vapor deposition (iCVD) is used to deposit conformal poly(hydroxyethyl methacrylate-co-ethylene glycol diacrylate) thin film electrolytes onto patterned Si-CNT composites structures. To complete the full cell, a slurry-based cathode is infiltrated into the patterned iCVD coated Si-CNT composite. This cell stack is then soaked in a liquid electrolyte and cycled, making this work the first demonstration of a 3D full cell fabricated using VA-CNTs and an iCVD electrolyte.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Planar lithium-ion cells with thick electrodes are often subject to an inherent tradeoff between energy and power density due to tortuous lithium-ion diffusion distances through the porous electrodes. Interdigitated 3D cell architectures circumvent this problem by incorporating thick electrode designs while also keeping lithium-ion diffusion distances short, thereby enabling cells with high energy and power densities. However, attempts to fabricate interdigitated cells have been hindered by difficulty in producing conformally coated electrolytes and incorporating the second electrode. Previously, we demonstrated that patterned vertically aligned carbon nanotubes (VA-CNTs) grown directly on Cu foil and coated with Si thin films could serve as a versatile template for high energy density 3D electrodes. Here, we investigate these Si-CNT composites as a template for 3D full cell design. Initiated chemical vapor deposition (iCVD) is used to deposit conformal poly(hydroxyethyl methacrylate-co-ethylene glycol diacrylate) thin film electrolytes onto patterned Si-CNT composites structures. To complete the full cell, a slurry-based cathode is infiltrated into the patterned iCVD coated Si-CNT composite. This cell stack is then soaked in a liquid electrolyte and cycled, making this work the first demonstration of a 3D full cell fabricated using VA-CNTs and an iCVD electrolyte.
10.
L Quincke, S Weinmann, J J Hinricher, M Galasso, C Althammer, F Kurnia, K J Kim, W Kiebach, J L M Rupp
Nanocrystalline LCO/LLZO Composite Cathode Films for Solid State Batteries Journal Article
In: Advanced Energy Materials, 2026, ISSN: 1614-6832.
@article{nokey,
title = {Nanocrystalline LCO/LLZO Composite Cathode Films for Solid State Batteries},
author = {L Quincke and S Weinmann and J J Hinricher and M Galasso and C Althammer and F Kurnia and K J Kim and W Kiebach and J L M Rupp},
url = {\<Go to ISI\>://WOS:001857933200001},
doi = {10.1002/aenm.71490},
issn = {1614-6832},
year = {2026},
date = {2026-08-25},
journal = {Advanced Energy Materials},
abstract = {Scalable fabrication of high-performing composite cathodes remains a key hurdle for oxide-based all-solid-state batteries (ASSBs). Li-garnet (Li7La3Zr2O12, LLZO) electrolytes provide high ionic conductivity and compatibility with lithium metal, yet, combining them with high-voltage layered oxides is often limited by high-temperature ceramic processing that complicates manufacturing and promotes interfacial side reactions. Here we report a LiCoO2/LLZO composite cathode prepared by single-solution spray deposition that co-deposits all constituents at a maximum processing temperature of 750 degrees C. The process produces dense, crack-free, micrometer-thick layers with nanograined, phase-separated microstructures. The two phases of cubic LLZO and layered LiCoO2 crystallize independently, only minor secondary phases form, and no cobalt migration into the LLZO substrate is detected. Consistent with a low cathode-electrolyte interfacial resistance observed after the first charge, full cells with lithium metal exhibit 111.7 mAh g-1 CAM initial discharge capacity and retain 93% of the capacity over 100 cycles. Capacity fade is dominated by progressive growth of cathode-electrolyte interfacial impedance, whereas post-mortem microscopy reveals preserved adhesion and morphology, suggesting the nanograined architecture accommodates cathode volume changes without severe cracking or delamination. Overall, single-solution co-deposition offers a practical, low-thermal-budget route to oxide composite cathodes and a scalable platform for extending LLZO-based ASSBs to broader cathode chemistries.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Scalable fabrication of high-performing composite cathodes remains a key hurdle for oxide-based all-solid-state batteries (ASSBs). Li-garnet (Li7La3Zr2O12, LLZO) electrolytes provide high ionic conductivity and compatibility with lithium metal, yet, combining them with high-voltage layered oxides is often limited by high-temperature ceramic processing that complicates manufacturing and promotes interfacial side reactions. Here we report a LiCoO2/LLZO composite cathode prepared by single-solution spray deposition that co-deposits all constituents at a maximum processing temperature of 750 degrees C. The process produces dense, crack-free, micrometer-thick layers with nanograined, phase-separated microstructures. The two phases of cubic LLZO and layered LiCoO2 crystallize independently, only minor secondary phases form, and no cobalt migration into the LLZO substrate is detected. Consistent with a low cathode-electrolyte interfacial resistance observed after the first charge, full cells with lithium metal exhibit 111.7 mAh g-1 CAM initial discharge capacity and retain 93% of the capacity over 100 cycles. Capacity fade is dominated by progressive growth of cathode-electrolyte interfacial impedance, whereas post-mortem microscopy reveals preserved adhesion and morphology, suggesting the nanograined architecture accommodates cathode volume changes without severe cracking or delamination. Overall, single-solution co-deposition offers a practical, low-thermal-budget route to oxide composite cathodes and a scalable platform for extending LLZO-based ASSBs to broader cathode chemistries.
9.
H Chu, T Defferriere, P Nandi, W Kaiser, L M Wolz, F Kurnia, K J Kim, W O'leary, T Altantzis, J Verbeeck, D A Egger, S Bals, J Eichhorn, H L Tuller, J L M Rupp
Charged grain boundaries limit short-circuit endurance in garnet solid-state battery electrolytes Journal Article
In: Nature Nanotechnology, vol. 21, no. 8, 2026, ISSN: 1748-3387.
@article{nokey,
title = {Charged grain boundaries limit short-circuit endurance in garnet solid-state battery electrolytes},
author = {H Chu and T Defferriere and P Nandi and W Kaiser and L M Wolz and F Kurnia and K J Kim and W O'leary and T Altantzis and J Verbeeck and D A Egger and S Bals and J Eichhorn and H L Tuller and J L M Rupp},
url = {\<Go to ISI\>://WOS:001812039400001},
doi = {10.1038/s41565-026-02206-0},
issn = {1748-3387},
year = {2026},
date = {2026-07-06},
journal = {Nature Nanotechnology},
volume = {21},
number = {8},
abstract = {Grain boundaries in lithium lanthanum zirconate solid-state electrolytes feature elevated electronic conduction and act as preferential sites for the nucleation of electrically isolated lithium metal during galvanostatic cycling in battery cells. However, the origin of local electronic conductivity variations remains unresolved. Here we show that lithium lanthanum zirconate grain boundaries carry ionic built-in charge, with lithium vacancies accumulating at the interface generating localized electric potentials (-0.15 V at 20 degrees C). This potential alters carrier distributions near the grain boundary, impeding ionic transport and increasing electronic conduction by a factor of 30 compared with bulk. This imbalance initiates internal lithium metal nucleation during cell operation and accelerates short-circuit failure. To mitigate charge build-up, we propose tailoring the processing oxygen activity and dopant stoichiometry, precisely tuning atomic-scale chemistry and interfacial potential. These modifications homogenize ionic transport and reduce electronic leakage, enabling the intrinsic critical current density to 1 mA cm-2. Our findings uncover how local defect landscapes shape charge transport and provide a pathway for chemically guided optimization of inorganic solid-state electrolytes at the nanoscale.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Grain boundaries in lithium lanthanum zirconate solid-state electrolytes feature elevated electronic conduction and act as preferential sites for the nucleation of electrically isolated lithium metal during galvanostatic cycling in battery cells. However, the origin of local electronic conductivity variations remains unresolved. Here we show that lithium lanthanum zirconate grain boundaries carry ionic built-in charge, with lithium vacancies accumulating at the interface generating localized electric potentials (-0.15 V at 20 degrees C). This potential alters carrier distributions near the grain boundary, impeding ionic transport and increasing electronic conduction by a factor of 30 compared with bulk. This imbalance initiates internal lithium metal nucleation during cell operation and accelerates short-circuit failure. To mitigate charge build-up, we propose tailoring the processing oxygen activity and dopant stoichiometry, precisely tuning atomic-scale chemistry and interfacial potential. These modifications homogenize ionic transport and reduce electronic leakage, enabling the intrinsic critical current density to 1 mA cm-2. Our findings uncover how local defect landscapes shape charge transport and provide a pathway for chemically guided optimization of inorganic solid-state electrolytes at the nanoscale.
8.
L Quincke, G Anand, F N Sayed, C P Grey, B J Lechner, J L M Rupp
The role of precursor decomposition in low-temperature solution-based synthesis and crystallization of Li-garnet solid electrolyte films Journal Article
In: Journal of Materials Chemistry A, 2026, ISSN: 2050-7488.
@article{nokey,
title = {The role of precursor decomposition in low-temperature solution-based synthesis and crystallization of Li-garnet solid electrolyte films},
author = {L Quincke and G Anand and F N Sayed and C P Grey and B J Lechner and J L M Rupp},
url = {\<Go to ISI\>://WOS:001772338100001},
doi = {10.1039/d6ta02188c},
issn = {2050-7488},
year = {2026},
date = {2026-05-22},
journal = {Journal of Materials Chemistry A},
abstract = {A key challenge for incorporation of oxide-based solid electrolytes into batteries remains the brittle nature of the ceramic, which makes scalable, low-cost fabrication of thin (\<20 \& micro;m) separators challenging. solution-based processing, involving the direct liquid-to-solid transformation of a precursor solution into a ceramic film through deposition and annealing, offers an attractive route to overcome these fabrication challenges while significantly reducing processing temperatures compared to conventional solid-state methods. However, the relationship between the initial choices made in precursor chemistries and the crystallization behavior remains poorly understood, limiting control over the phase formation process. Here, we investigate how the precursor decompositions influence the structure evolution during annealing and crystallization of solution-processed Li-garnet solid electrolyte films. The results reveal a sequence of solvent and precursor decompositions with the Li-precursor, LiNO3, decomposition occurring last and in parallel with the nucleation of La2Zr2O7 as the first crystalline metal-oxide phase. Upon Li-precursor decomposition, the latter is lithiated to form the desired highly conductive cubic Li6.25Al0.25La3Zr2O12 phase. This simultaneity of crystallization and decomposition events demonstrates the importance of the initial precursor choices to control the crystallization process. Through this work, we contribute to fundamental ceramic materials science by establishing a systematic methodology for studying solution-processing and providing a foundation for future precursor design of next-generation solid electrolyte battery components.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
A key challenge for incorporation of oxide-based solid electrolytes into batteries remains the brittle nature of the ceramic, which makes scalable, low-cost fabrication of thin (<20 & micro;m) separators challenging. solution-based processing, involving the direct liquid-to-solid transformation of a precursor solution into a ceramic film through deposition and annealing, offers an attractive route to overcome these fabrication challenges while significantly reducing processing temperatures compared to conventional solid-state methods. However, the relationship between the initial choices made in precursor chemistries and the crystallization behavior remains poorly understood, limiting control over the phase formation process. Here, we investigate how the precursor decompositions influence the structure evolution during annealing and crystallization of solution-processed Li-garnet solid electrolyte films. The results reveal a sequence of solvent and precursor decompositions with the Li-precursor, LiNO3, decomposition occurring last and in parallel with the nucleation of La2Zr2O7 as the first crystalline metal-oxide phase. Upon Li-precursor decomposition, the latter is lithiated to form the desired highly conductive cubic Li6.25Al0.25La3Zr2O12 phase. This simultaneity of crystallization and decomposition events demonstrates the importance of the initial precursor choices to control the crystallization process. Through this work, we contribute to fundamental ceramic materials science by establishing a systematic methodology for studying solution-processing and providing a foundation for future precursor design of next-generation solid electrolyte battery components.
7.
J J Hinricher, K P Sokol, P Simons, K J Kim, M Foshey, Y S Tian, T Prein, L J Miara, E Olivetti, W Matusik, J L M Rupp
Roadmap for High-Throughput Ceramic Materials Synthesis and Discovery for Batteries Journal Article
In: Advanced Energy Materials, 2026, ISSN: 1614-6832.
@article{nokey,
title = {Roadmap for High-Throughput Ceramic Materials Synthesis and Discovery for Batteries},
author = {J J Hinricher and K P Sokol and P Simons and K J Kim and M Foshey and Y S Tian and T Prein and L J Miara and E Olivetti and W Matusik and J L M Rupp},
url = {\<Go to ISI\>://WOS:001723315900001},
doi = {10.1002/aenm.202506213},
issn = {1614-6832},
year = {2026},
date = {2026-03-25},
journal = {Advanced Energy Materials},
abstract = {Global energy demand is projected to grow 30% within the next three decades, driven primarily by population growth and urbanization, leading to greater material needs in energy, and necessitates a new regime of accelerated research via a fundamentally improved strategy. In this perspective, we examine traditional ceramic synthesis methods for high-throughput synthesis and optimization, and highlight requirements and opportunities of synthesis routes for rapid alterations in the future. Such a strategy relies on flexible direct liquid precursor-to-solid film methods rather than traditional, but slower, solid-state methods. Application of computer-aided decision making takes in variables at all levels of fabrication and operates on both material and device characteristics to initialize and optimize the search for higher-performance devices, not just narrow materials optimization. Collectively, we provide a blueprint for accelerated ceramic materials and device improvements of next-generation materials research targeting energy storage.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Global energy demand is projected to grow 30% within the next three decades, driven primarily by population growth and urbanization, leading to greater material needs in energy, and necessitates a new regime of accelerated research via a fundamentally improved strategy. In this perspective, we examine traditional ceramic synthesis methods for high-throughput synthesis and optimization, and highlight requirements and opportunities of synthesis routes for rapid alterations in the future. Such a strategy relies on flexible direct liquid precursor-to-solid film methods rather than traditional, but slower, solid-state methods. Application of computer-aided decision making takes in variables at all levels of fabrication and operates on both material and device characteristics to initialize and optimize the search for higher-performance devices, not just narrow materials optimization. Collectively, we provide a blueprint for accelerated ceramic materials and device improvements of next-generation materials research targeting energy storage.
6.
A Singh, D Blätte, R Guntermann, L Quincke, J L M Rupp, T Bein
Tuning Redox Behavior of Pyrene-Benzothiadiazole/TTF-Based Covalent Organic Framework Electrodes in Dual-Ion Batteries Journal Article
In: Angewandte Chemie-International Edition, vol. 65, no. 12, 2026, ISSN: 1433-7851.
@article{nokey,
title = {Tuning Redox Behavior of Pyrene-Benzothiadiazole/TTF-Based Covalent Organic Framework Electrodes in Dual-Ion Batteries},
author = {A Singh and D Bl\"{a}tte and R Guntermann and L Quincke and J L M Rupp and T Bein},
url = {\<Go to ISI\>://WOS:001684893800001},
doi = {10.1002/anie.202522720},
issn = {1433-7851},
year = {2026},
date = {2026-03-16},
journal = {Angewandte Chemie-International Edition},
volume = {65},
number = {12},
abstract = {Covalent organic frameworks (COFs) have emerged as promising electrode materials for secondary-ion batteries, where redox-active building blocks and linkages enable tunable redox properties, while ordered pores serve as nanochannels for fast ion transport. We report a novel highly crystalline 2D PyTTF-COF, synthesized by integrating n-type pyrene-benzothiadiazole (PyBT) and p-type tetrathiafulvalene (TTF) subunits via an n-type imine linkage, yielding a bipolar electrode capable of reversible 16 e- dual cation-anion storage. Initially, the dual-ion, redox synergy was tested in a Li-ion half-cell, where PyTTF served as cathode, and 1 \& mcy; LiPF6 or LiTFSI electrolytes were employed to probe anion-dependent electrochemical behavior. Electrochemical evaluation in Li-ion half cells revealed a wide electrochemical window of 0.1-3.6 V vs. Li/Li+, with markedly enhanced charge-storage kinetics and ion diffusion with LiTFSI relative to LiPF6 electrolytes. The PyTTF electrode delivered specific capacities of 286 mAh g-1 (LiTFSI) and 184 mAh g-1 (LiPF6) at 0.3 A g-1, highlighting the strong influence of anion identity. Systematic variation of LiTFSI salt concentration (1-3 \& mcy;) revealed strong correlations between electrolyte composition, ion storage dynamics, and interfacial charge-transfer resistance. This study highlights, for the first time, the critical importance of tailoring both charge-carrier identity and electrolyte concentration to unlock the full potential of bipolar COF electrodes for dual-ion batteries.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Covalent organic frameworks (COFs) have emerged as promising electrode materials for secondary-ion batteries, where redox-active building blocks and linkages enable tunable redox properties, while ordered pores serve as nanochannels for fast ion transport. We report a novel highly crystalline 2D PyTTF-COF, synthesized by integrating n-type pyrene-benzothiadiazole (PyBT) and p-type tetrathiafulvalene (TTF) subunits via an n-type imine linkage, yielding a bipolar electrode capable of reversible 16 e- dual cation-anion storage. Initially, the dual-ion, redox synergy was tested in a Li-ion half-cell, where PyTTF served as cathode, and 1 & mcy; LiPF6 or LiTFSI electrolytes were employed to probe anion-dependent electrochemical behavior. Electrochemical evaluation in Li-ion half cells revealed a wide electrochemical window of 0.1-3.6 V vs. Li/Li+, with markedly enhanced charge-storage kinetics and ion diffusion with LiTFSI relative to LiPF6 electrolytes. The PyTTF electrode delivered specific capacities of 286 mAh g-1 (LiTFSI) and 184 mAh g-1 (LiPF6) at 0.3 A g-1, highlighting the strong influence of anion identity. Systematic variation of LiTFSI salt concentration (1-3 & mcy;) revealed strong correlations between electrolyte composition, ion storage dynamics, and interfacial charge-transfer resistance. This study highlights, for the first time, the critical importance of tailoring both charge-carrier identity and electrolyte concentration to unlock the full potential of bipolar COF electrodes for dual-ion batteries.
5.
S Weinmann, L Quincke, L Winkler, J J Hinricher, F Kurnia, K J Kim, J L M Rupp
Sustainable functional ceramics Journal Article
In: Nature Nanotechnology, vol. 20, no. 12, pp. 1729-1745, 2025, ISSN: 1748-3387.
@article{nokey,
title = {Sustainable functional ceramics},
author = {S Weinmann and L Quincke and L Winkler and J J Hinricher and F Kurnia and K J Kim and J L M Rupp},
url = {\<Go to ISI\>://WOS:001637004800001},
doi = {10.1038/s41565-025-02076-y},
issn = {1748-3387},
year = {2025},
date = {2025-12-20},
journal = {Nature Nanotechnology},
volume = {20},
number = {12},
pages = {1729-1745},
abstract = {The rapid rise of functional ceramics across various sectors, including electronics, energy storage and automotive, is projected to drive annual growth rates of up to 35% until 2030. With this significant growth, the substantial energy required for mining and ceramic manufacturing leads to notable greenhouse gas emissions. In this Review, we discuss measures to enhance the sustainability of functional ceramic materials, including low-energy and low-CO2 production methods. We evaluate their potential impact and technology readiness for functional ceramics with different nanoscale architectures and varying levels of structural and chemical complexity across diverse fields. We examine end-of-life recycling strategies and assess the role of critical raw materials in both established and rapidly growing markets, concluding with a discussion of supporting policy measures. Through this work, we propose a tangible action plan to lower CO2-equivalent emissions in producing future functional ceramics, whether through synthesis techniques, manufacturing tools, densification processes, or chemical and reaction protocols. This provides a blueprint for designing and manufacturing the next generation of more sustainable functional ceramic materials.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The rapid rise of functional ceramics across various sectors, including electronics, energy storage and automotive, is projected to drive annual growth rates of up to 35% until 2030. With this significant growth, the substantial energy required for mining and ceramic manufacturing leads to notable greenhouse gas emissions. In this Review, we discuss measures to enhance the sustainability of functional ceramic materials, including low-energy and low-CO2 production methods. We evaluate their potential impact and technology readiness for functional ceramics with different nanoscale architectures and varying levels of structural and chemical complexity across diverse fields. We examine end-of-life recycling strategies and assess the role of critical raw materials in both established and rapidly growing markets, concluding with a discussion of supporting policy measures. Through this work, we propose a tangible action plan to lower CO2-equivalent emissions in producing future functional ceramics, whether through synthesis techniques, manufacturing tools, densification processes, or chemical and reaction protocols. This provides a blueprint for designing and manufacturing the next generation of more sustainable functional ceramic materials.
4.
L P Kong, P J Williams, F Brushett, J L M Rupp
Unveiling Coexisting Battery-Type and Pseudocapacitive Intercalation Mechanisms in Lithium Titanate Journal Article
In: Advanced Energy Materials, 2025, ISSN: 1614-6832.
@article{nokey,
title = {Unveiling Coexisting Battery-Type and Pseudocapacitive Intercalation Mechanisms in Lithium Titanate},
author = {L P Kong and P J Williams and F Brushett and J L M Rupp},
url = {\<Go to ISI\>://WOS:001544773300001},
doi = {10.1002/aenm.202503080},
issn = {1614-6832},
year = {2025},
date = {2025-08-06},
journal = {Advanced Energy Materials},
abstract = {Conventional lithium-ion (Li-ion) batteries and supercapacitors face inherent trade-offs between power and energy densities, restricting their adaptability in applications requiring dynamic performance across both regimes. Here, a "zero-strain" lithium titanate (Li4Ti5O12) as a new class of battery-capacitive material exhibiting dual lithiation mechanisms, combining diffusion-controlled battery-type redox reactions and surface-controlled pseudocapacitive intercalation, depending on the operating potential, is revealed. At approximate to 1.55 V (vs Li/Li+), lithium titanate undergoes a two-phase transition reaction between Li4Ti5O12 and Li7Ti5O12, involving Li migration between 8a and 16c Wyckoff sites. Upon deeper lithiation to potentials near 0 V, Li ions reoccupy the 8a sites, triggering a reversible pseudocapacitive response with fast kinetics. Leveraging these dual lithiation mechanisms, lithium titanate delivers a high reversible capacity of approximate to 215 mAh g-1 at 20 mA g-1, retaining 148 mAh g-1 at 2000 mA g-1. The high-rate capability and cycling stability are attributed to a unique structure with minimal lattice strain during Li-site occupation. This work presents the first clear demonstration of a unique dual-mode charge storage mechanism in lithium titanate, which can reversibly operate in either battery-type or pseudocapacitive regimes.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Conventional lithium-ion (Li-ion) batteries and supercapacitors face inherent trade-offs between power and energy densities, restricting their adaptability in applications requiring dynamic performance across both regimes. Here, a "zero-strain" lithium titanate (Li4Ti5O12) as a new class of battery-capacitive material exhibiting dual lithiation mechanisms, combining diffusion-controlled battery-type redox reactions and surface-controlled pseudocapacitive intercalation, depending on the operating potential, is revealed. At approximate to 1.55 V (vs Li/Li+), lithium titanate undergoes a two-phase transition reaction between Li4Ti5O12 and Li7Ti5O12, involving Li migration between 8a and 16c Wyckoff sites. Upon deeper lithiation to potentials near 0 V, Li ions reoccupy the 8a sites, triggering a reversible pseudocapacitive response with fast kinetics. Leveraging these dual lithiation mechanisms, lithium titanate delivers a high reversible capacity of approximate to 215 mAh g-1 at 20 mA g-1, retaining 148 mAh g-1 at 2000 mA g-1. The high-rate capability and cycling stability are attributed to a unique structure with minimal lattice strain during Li-site occupation. This work presents the first clear demonstration of a unique dual-mode charge storage mechanism in lithium titanate, which can reversibly operate in either battery-type or pseudocapacitive regimes.
3.
M Munjal, T Prein, M M Ramadan, H B Smith, V Venugopal, J L M Rupp, I I Abate, E A Olivetti, K J Huang
Process cost analysis of performance challenges and their mitigations in sodium-ion battery cathode materials Journal Article
In: Joule, pp. 101871, 2025, ISSN: 2542-4351.
@article{nokey,
title = {Process cost analysis of performance challenges and their mitigations in sodium-ion battery cathode materials},
author = {M Munjal and T Prein and M M Ramadan and H B Smith and V Venugopal and J L M Rupp and I I Abate and E A Olivetti and K J Huang},
url = {https://www.sciencedirect.com/science/article/pii/S2542435125000522},
doi = {https://doi.org/10.1016/j.joule.2025.101871},
issn = {2542-4351},
year = {2025},
date = {2025-03-14},
journal = {Joule},
pages = {101871},
abstract = {Summary The success of sodium-ion batteries (SIBs) hinges on mitigating underperformance in ways that are cost effective, manufacturable, and scalable. This work investigates interfacial, morphological, and bulk interventions to enhance the performance of layered metal oxide cathode active materials (CAMs) for SIBs. We mapped the full space of literature-reported SIB CAM challenges and their mitigations. We then estimated the manufacturing costs for a diverse and representative set of mitigation approaches. Adding sacrificial salts can be cost effective, given low materials costs and minimal process changes. By contrast, many methods are reported to tune CAM morphology. Several are likely challenging at scale due to process throughput and yield limitations. Finally, bulk modifications can mitigate the moisture sensitivity of some CAMs, a likely less costly route than expanding stringent atmosphere controls during manufacturing. We end by discussing the limits and promise of process cost analysis, given the current state of battery reporting in the literature.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Summary The success of sodium-ion batteries (SIBs) hinges on mitigating underperformance in ways that are cost effective, manufacturable, and scalable. This work investigates interfacial, morphological, and bulk interventions to enhance the performance of layered metal oxide cathode active materials (CAMs) for SIBs. We mapped the full space of literature-reported SIB CAM challenges and their mitigations. We then estimated the manufacturing costs for a diverse and representative set of mitigation approaches. Adding sacrificial salts can be cost effective, given low materials costs and minimal process changes. By contrast, many methods are reported to tune CAM morphology. Several are likely challenging at scale due to process throughput and yield limitations. Finally, bulk modifications can mitigate the moisture sensitivity of some CAMs, a likely less costly route than expanding stringent atmosphere controls during manufacturing. We end by discussing the limits and promise of process cost analysis, given the current state of battery reporting in the literature.
2.
S C Sand, J L M Rupp, B Yildiz
A critical review on Li-ion transport, chemistry and structure of ceramic–polymer composite electrolytes for solid state batteries Journal Article
In: Chemical Society Reviews, vol. 54, no. 1, pp. 178-200, 2024, ISSN: 0306-0012.
@article{nokey,
title = {A critical review on Li-ion transport, chemistry and structure of ceramic\textendashpolymer composite electrolytes for solid state batteries},
author = {S C Sand and J L M Rupp and B Yildiz},
url = {http://dx.doi.org/10.1039/D4CS00214H},
doi = {10.1039/D4CS00214H},
issn = {0306-0012},
year = {2024},
date = {2024-11-18},
journal = {Chemical Society Reviews},
volume = {54},
number = {1},
pages = {178-200},
abstract = {In the transition to safer, more energy-dense solid state batteries, polymer\textendashceramic composite electrolytes may offer a potential route to achieve simultaneously high Li-ion conductivity and enhanced mechanical stability. Despite numerous studies on the polymer\textendashceramic composite electrolytes, disagreements persist on whether the polymer or the ceramic is positively impacted in their constituent ionic conductivity for such composite electrolytes, and even whether the interface is a blocking layer or a highly conductive lithium ion path. This lack of understanding limits the design of effective composite solid electrolytes. By thorough and critical analysis of the data collected in the field over the last three decades, we present arguments for lithium conduction through the bulk of the polymer, ceramic, or their interface. From this analysis, we can conclude that the unexpectedly high conductivity reported for some ceramic\textendashpolymer composites cannot be accounted for by the ceramic phase alone. There is evidence to support the theory that the Li-ion conductivity in the polymer phase increases along this interface in contact with the ceramic. The potential mechanisms for this include increased free volume, decreased crystallinity, and modulated Lewis acid\textendashbase effects in the polymer, with the former two to be the more likely mechanisms. Future work in this field requires understanding these factors more quantitatively, and tuning of the ceramic surface chemistry and morphology in order to obtain targeted structural modifications in the polymer phase.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
In the transition to safer, more energy-dense solid state batteries, polymer–ceramic composite electrolytes may offer a potential route to achieve simultaneously high Li-ion conductivity and enhanced mechanical stability. Despite numerous studies on the polymer–ceramic composite electrolytes, disagreements persist on whether the polymer or the ceramic is positively impacted in their constituent ionic conductivity for such composite electrolytes, and even whether the interface is a blocking layer or a highly conductive lithium ion path. This lack of understanding limits the design of effective composite solid electrolytes. By thorough and critical analysis of the data collected in the field over the last three decades, we present arguments for lithium conduction through the bulk of the polymer, ceramic, or their interface. From this analysis, we can conclude that the unexpectedly high conductivity reported for some ceramic–polymer composites cannot be accounted for by the ceramic phase alone. There is evidence to support the theory that the Li-ion conductivity in the polymer phase increases along this interface in contact with the ceramic. The potential mechanisms for this include increased free volume, decreased crystallinity, and modulated Lewis acid–base effects in the polymer, with the former two to be the more likely mechanisms. Future work in this field requires understanding these factors more quantitatively, and tuning of the ceramic surface chemistry and morphology in order to obtain targeted structural modifications in the polymer phase.
1.
W O’leary, M Grumet, W Kaiser, T Bučko, J L M Rupp, D A Egger
In: Journal of the American Chemical Society, vol. 146, no. 39, pp. 26863-26876, 2024, ISSN: 0002-7863.
@article{nokey,
title = {Rapid Characterization of Point Defects in Solid-State Ion Conductors Using Raman Spectroscopy, Machine-Learning Force Fields, and Atomic Raman Tensors},
author = {W O’leary and M Grumet and W Kaiser and T Bu\v{c}ko and J L M Rupp and D A Egger},
url = {https://doi.org/10.1021/jacs.4c07812},
doi = {10.1021/jacs.4c07812},
issn = {0002-7863},
year = {2024},
date = {2024-10-02},
journal = {Journal of the American Chemical Society},
volume = {146},
number = {39},
pages = {26863-26876},
abstract = {The successful design of solid-state photo- and electrochemical devices depends on the careful engineering of point defects in solid-state ion conductors. Characterization of point defects is critical to these efforts, but the best-developed techniques are difficult and time-consuming. Raman spectroscopy─with its exceptional speed, flexibility, and accessibility─is a promising alternative. Raman signatures arise from point defects due to local symmetry breaking and structural distortions. Unfortunately, the assignment of these signatures is often hampered by a shortage of reference compounds and corresponding reference spectra. This issue can be circumvented by calculation of defect-induced Raman signatures from first principles, but this is computationally demanding. Here, we introduce an efficient computational procedure for the prediction of point defect Raman signatures in solid-state ion conductors. Our method leverages machine-learning force fields and “atomic Raman tensors”, i.e., polarizability fluctuations due to motions of individual atoms. We find that our procedure reduces computational cost by up to 80% compared to existing first-principles frozen-phonon approaches. These efficiency gains enable synergistic computational\textendashexperimental investigations, in our case allowing us to precisely interpret the Raman spectra of Sr(Ti0.94Ni0.06)O3-δ, a model oxygen ion conductor. By predicting Raman signatures of specific point defects, we determine the nature of dominant defects and unravel impacts of temperature and quenching on in situ and ex situ Raman spectra. Specifically, our findings reveal the temperature-dependent distribution and association behavior of oxygen vacancies and nickel substitutional defects. Overall, our approach enables rapid Raman-based characterization of point defects to support defect engineering in novel solid-state ion conductors.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The successful design of solid-state photo- and electrochemical devices depends on the careful engineering of point defects in solid-state ion conductors. Characterization of point defects is critical to these efforts, but the best-developed techniques are difficult and time-consuming. Raman spectroscopy─with its exceptional speed, flexibility, and accessibility─is a promising alternative. Raman signatures arise from point defects due to local symmetry breaking and structural distortions. Unfortunately, the assignment of these signatures is often hampered by a shortage of reference compounds and corresponding reference spectra. This issue can be circumvented by calculation of defect-induced Raman signatures from first principles, but this is computationally demanding. Here, we introduce an efficient computational procedure for the prediction of point defect Raman signatures in solid-state ion conductors. Our method leverages machine-learning force fields and “atomic Raman tensors”, i.e., polarizability fluctuations due to motions of individual atoms. We find that our procedure reduces computational cost by up to 80% compared to existing first-principles frozen-phonon approaches. These efficiency gains enable synergistic computational–experimental investigations, in our case allowing us to precisely interpret the Raman spectra of Sr(Ti0.94Ni0.06)O3-δ, a model oxygen ion conductor. By predicting Raman signatures of specific point defects, we determine the nature of dominant defects and unravel impacts of temperature and quenching on in situ and ex situ Raman spectra. Specifically, our findings reveal the temperature-dependent distribution and association behavior of oxygen vacancies and nickel substitutional defects. Overall, our approach enables rapid Raman-based characterization of point defects to support defect engineering in novel solid-state ion conductors.