Sushil Shivaji Sangale, Sunil Vinod Barma, Sung-Nam Kwon, Shi-Joon Sung, Dae-Hwan Kim, Sae Byeok Jo, Seok-In Na
Perovskite solar cells (PSCs) have emerged as leading candidates for next-generation photovoltaics; however, translating laboratory-scale efficiencies to industrial production remains limited by key challenges such as achieving high-quality film and addressing solvent toxicity. To overcome these limitations, we formulate colloidal ink by incorporating iodobenzene (Iodo) as an environmentally sustainable additive into a DMSO-based system, enabling scalable film fabrication via slot-die coating. It is found that Iodo-based additives enhance wettability, facilitate the formation of larger colloidal particles, and enable controlled solidification through solvent evaporation kinetics. Specifically, the inclusion of Iodo modulates colloidal size and evaporation behavior, which in turn reduces the effective nucleation barrier and promotes directional grain growth. This leads to the formation of dense, uniform films with improved crystallinity and minimal defects. Devices fabricated using Iodo-based ink achieved an efficiency of up to 22.3% (the highest reported efficiency in a highly toxic DMF-free system), encapsulated devices retaining 85% of their initial value after 1200 h of maximum power point tracking (MPPT) and 77% after 8400 h (unencapsulated devices stored in the dark), demonstrating excellent operational and long-term stability. Furthermore, the DMF-free, DMSO-based ink shows excellent scalability, achieving efficiencies of 21% and 19.5% for 2.7 and 31.50 cm2 modules, respectively.
{"title":"Greener Colloidal Ink Engineering and Local Solidification Control for High-Performance Slot-Die Coated Perovskite Solar Modules","authors":"Sushil Shivaji Sangale, Sunil Vinod Barma, Sung-Nam Kwon, Shi-Joon Sung, Dae-Hwan Kim, Sae Byeok Jo, Seok-In Na","doi":"10.1002/aenm.202504928","DOIUrl":"https://doi.org/10.1002/aenm.202504928","url":null,"abstract":"Perovskite solar cells (PSCs) have emerged as leading candidates for next-generation photovoltaics; however, translating laboratory-scale efficiencies to industrial production remains limited by key challenges such as achieving high-quality film and addressing solvent toxicity. To overcome these limitations, we formulate colloidal ink by incorporating iodobenzene (Iodo) as an environmentally sustainable additive into a DMSO-based system, enabling scalable film fabrication via slot-die coating. It is found that Iodo-based additives enhance wettability, facilitate the formation of larger colloidal particles, and enable controlled solidification through solvent evaporation kinetics. Specifically, the inclusion of Iodo modulates colloidal size and evaporation behavior, which in turn reduces the effective nucleation barrier and promotes directional grain growth. This leads to the formation of dense, uniform films with improved crystallinity and minimal defects. Devices fabricated using Iodo-based ink achieved an efficiency of up to 22.3% (the highest reported efficiency in a highly toxic DMF-free system), encapsulated devices retaining 85% of their initial value after 1200 h of maximum power point tracking (MPPT) and 77% after 8400 h (unencapsulated devices stored in the dark), demonstrating excellent operational and long-term stability. Furthermore, the DMF-free, DMSO-based ink shows excellent scalability, achieving efficiencies of 21% and 19.5% for 2.7 and 31.50 cm<sup>2</sup> modules, respectively.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"70 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Balancing stability and activity of the hydrogen evolution reaction (HER) electrocatalysis remains challenging for advanced electrolysis technologies. This work introduces a synergistic design strategy to tackle the challenge with in situ surface restructuring. Fe-based double perovskite is developed with an optimal electronic structure for HER catalysis, delivering an overpotential of 325 mV in 0.1 m KOH and 184 mV in 1 m KOH at 10 mA/cm2, among the best reported. Additionally, the catalyst exhibited remarkable self-improving stability, with specific activity increasing 1.98 times at 300 mV overpotential after 20 h, due to the restructuring of an amorphous layer confirmed with transmission electron microscopy. To demonstrate practical utility, the catalyst was integrated into an active flow membraneless electrolyzer (AFME), a promising technology that is currently limited by instability. The device demonstrated outstanding operational stability for 1000 h at 50 mA/cm2, with a minimal decay rate of 0.25 mV/h, establishing a new benchmark for membraneless systems. This work not only presents a powerful strategy for designing self-improving catalysts but also validates its practical efficacy in next generation electrolyzer technologies, paving the way for cost-effective green hydrogen production.
{"title":"Compositional Tuning and Surface Restructuring Synergistically Enhance Perovskite Ferrite Catalysts for Hydrogen Evolution in a Membrane-Less Electrolyzer","authors":"Yixin Bi, Yuhao Wang, Zilong Wang, Yufei Song, Nuotong Li, Jingwei Li, Arini Kar, Qing Chen, Francesco Ciucci","doi":"10.1002/aenm.202505486","DOIUrl":"https://doi.org/10.1002/aenm.202505486","url":null,"abstract":"Balancing stability and activity of the hydrogen evolution reaction (HER) electrocatalysis remains challenging for advanced electrolysis technologies. This work introduces a synergistic design strategy to tackle the challenge with in situ surface restructuring. Fe-based double perovskite is developed with an optimal electronic structure for HER catalysis, delivering an overpotential of 325 mV in 0.1 <span>m</span> KOH and 184 mV in 1 <span>m</span> KOH at 10 mA/cm<sup>2</sup>, among the best reported. Additionally, the catalyst exhibited remarkable self-improving stability, with specific activity increasing 1.98 times at 300 mV overpotential after 20 h, due to the restructuring of an amorphous layer confirmed with transmission electron microscopy. To demonstrate practical utility, the catalyst was integrated into an active flow membraneless electrolyzer (AFME), a promising technology that is currently limited by instability. The device demonstrated outstanding operational stability for 1000 h at 50 mA/cm<sup>2</sup>, with a minimal decay rate of 0.25 mV/h, establishing a new benchmark for membraneless systems. This work not only presents a powerful strategy for designing self-improving catalysts but also validates its practical efficacy in next generation electrolyzer technologies, paving the way for cost-effective green hydrogen production.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"295 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138860","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sung Jae Jeon, Nam Gyu Yang, Ji Youn Kim, Eunkyung Cho, Jeewon Park, Geonheon Lee, Changduk Yang, Doo Kyung Moon
Achieving high efficiency and long-term stability under ambient processing conditions remains a critical hurdle for the commercialization of organic solar cells (OSCs). Here, we report two new Y6-analogs—BT(BO)-v-T(C12)-4F (4F) and BT(BO)-v-T(C12)-4Cl (4Cl)—featuring vinylene (v)-bridged DA′D cores, designed to improve the material's scalability while maintaining the structural advantages of Y6-type acceptors. Morphological and device-level investigations reveal that these M-Y6 derivatives facilitate thermodynamically stable molecular packing and favorable crystalline orientation, even when fully processed in air. Incorporation of 4F into a layer-by-layer ternary architecture with D18/L8-BO via a reproducible air-processing protocol results in a certified power conversion efficiency (PCE) of 19%, among the highest reported for conventional OSCs fabricated under ambient conditions. Moreover, 4F-based devices demonstrate exceptional thermal and photostability, retaining over 80% of their initial PCE after extended aging under the ISOS-L-1 protocol without encapsulation. These improvements are attributed to the enhanced crystallinity, vertical molecular alignment, and morphological robustness imparted by the 4F acceptor. This study identifies BT(BO)-v-T(C12)-4F as a promising air-processable acceptor for scalable OSCs that combine high efficiency with long-term operational durability.
{"title":"Streamlined Y6-Analogs Enabling Efficient Ambient-Air-Processed Organic Solar Cells","authors":"Sung Jae Jeon, Nam Gyu Yang, Ji Youn Kim, Eunkyung Cho, Jeewon Park, Geonheon Lee, Changduk Yang, Doo Kyung Moon","doi":"10.1002/aenm.202505110","DOIUrl":"https://doi.org/10.1002/aenm.202505110","url":null,"abstract":"Achieving high efficiency and long-term stability under ambient processing conditions remains a critical hurdle for the commercialization of organic solar cells (OSCs). Here, we report two new Y6-analogs—BT(BO)-<i>v</i>-T(C12)-4F (4F) and BT(BO)-<i>v</i>-T(C12)-4Cl (4Cl)—featuring vinylene (<i>v</i>)-bridged DA′D cores, designed to improve the material's scalability while maintaining the structural advantages of Y6-type acceptors. Morphological and device-level investigations reveal that these M-Y6 derivatives facilitate thermodynamically stable molecular packing and favorable crystalline orientation, even when fully processed in air. Incorporation of 4F into a layer-by-layer ternary architecture with D18/L8-BO via a reproducible air-processing protocol results in a certified power conversion efficiency (PCE) of 19%, among the highest reported for conventional OSCs fabricated under ambient conditions. Moreover, 4F-based devices demonstrate exceptional thermal and photostability, retaining over 80% of their initial PCE after extended aging under the ISOS-L-1 protocol without encapsulation. These improvements are attributed to the enhanced crystallinity, vertical molecular alignment, and morphological robustness imparted by the 4F acceptor. This study identifies BT(BO)-<i>v</i>-T(C12)-4F as a promising air-processable acceptor for scalable OSCs that combine high efficiency with long-term operational durability.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"132 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138857","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuexin Liu, Tianyu Zhang, Zian Li, Zhongqing Ma, Yong Hu
Aqueous zinc-ion batteries (AZIBs) are promising candidates for large-scale energy storage due to their intrinsic safety and low cost. However, their commercialization is hampered by notorious zinc anode issues, including uncontrolled dendrite growth and parasitic side reactions. Multiscale interfacial regulation has recently emerged as a transformative strategy to address these challenges. This approach overcomes the limitations of single-interface modulation by constructing multilayer structures and optimizing interface coupling, thereby providing effective anode protection. To promote uniform zinc plating and suppress side reactions, this review comprehensively summarizes multiscale strategies that span the optimization of multi-physical fields, zinc deposition orientation, and electrolyte solvation structures. We systematically present recent advances in applying these multiscale strategies to zinc foil, zinc powder, and host-based anodes, as well as separators and hydrogel electrolytes, with a focus on their design principles, underlying mechanisms, and scenario-specific applicability. Furthermore, we elucidate how this technology achieves synergistic optimization of ion transport, deposition behavior, and the interfacial environment through functionally complementary multilayer, Janus, or gradient interfaces, thereby systematically mitigating zinc anode failure. Finally, future research directions and challenges are discussed, emphasizing that a profound mechanistic understanding coupled with rational design is pivotal for unlocking the full potential of next-generation AZIBs.
{"title":"Multiscale Interfacial Regulation for Stable Zinc Anodes: From Fundamental Mechanisms to Practical Applications","authors":"Yuexin Liu, Tianyu Zhang, Zian Li, Zhongqing Ma, Yong Hu","doi":"10.1002/aenm.70704","DOIUrl":"https://doi.org/10.1002/aenm.70704","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) are promising candidates for large-scale energy storage due to their intrinsic safety and low cost. However, their commercialization is hampered by notorious zinc anode issues, including uncontrolled dendrite growth and parasitic side reactions. Multiscale interfacial regulation has recently emerged as a transformative strategy to address these challenges. This approach overcomes the limitations of single-interface modulation by constructing multilayer structures and optimizing interface coupling, thereby providing effective anode protection. To promote uniform zinc plating and suppress side reactions, this review comprehensively summarizes multiscale strategies that span the optimization of multi-physical fields, zinc deposition orientation, and electrolyte solvation structures. We systematically present recent advances in applying these multiscale strategies to zinc foil, zinc powder, and host-based anodes, as well as separators and hydrogel electrolytes, with a focus on their design principles, underlying mechanisms, and scenario-specific applicability. Furthermore, we elucidate how this technology achieves synergistic optimization of ion transport, deposition behavior, and the interfacial environment through functionally complementary multilayer, Janus, or gradient interfaces, thereby systematically mitigating zinc anode failure. Finally, future research directions and challenges are discussed, emphasizing that a profound mechanistic understanding coupled with rational design is pivotal for unlocking the full potential of next-generation AZIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"5 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138859","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jianxin Deng, Xingai Wang, Hong Lu, Bin Tang, Xihua Wang, Jinlin Li, Zhen Zhou, Honghui Gu, Haichang Zhang, Fei Ding
With the expanding applications of lithium-ion batteries (LIBs), there is a growing demand for high-performance LIBs with high-temperature-resistant, especially in fields such as military or aerospace exploration. However, traditional electrolytes suffer from poor thermal stability and severe side reactions at temperatures above 60°C, failing to meet the practical use under high-temperature conditions. Here, we propose a high-temperature-resistant electrolyte system, i.e., high-boiling-point propylene carbonate, as well as dual-anion engineering to improve interface stability. The anion-regulated solvation structures achieve perfect compatibility between propylene carbonate and graphite, while the dual-anion synergy induces the formation of organic/inorganic gradient interphase dominated by C-F/LiBxOy species under high temperature. The LiNi0.8Co0.1Mn0.1O2 || graphite pouch cells demonstrate excellent cycling durability and rate capability under extreme conditions, achieving an outstanding lifespan of over 1000 cycles at 100°C, while retaining 55.7% of their rated capacity under a harsh 100°C and 5 C condition. Remarkably, the cells maintain normal electrochemical functionality even at 150°C, underscoring the robustness of the proposed electrolyte design.
{"title":"Functionalized and Customized Electrolyte Enabling NCM811||Gr Pouch Cells Operation at 150°C","authors":"Jianxin Deng, Xingai Wang, Hong Lu, Bin Tang, Xihua Wang, Jinlin Li, Zhen Zhou, Honghui Gu, Haichang Zhang, Fei Ding","doi":"10.1002/aenm.70718","DOIUrl":"https://doi.org/10.1002/aenm.70718","url":null,"abstract":"With the expanding applications of lithium-ion batteries (LIBs), there is a growing demand for high-performance LIBs with high-temperature-resistant, especially in fields such as military or aerospace exploration. However, traditional electrolytes suffer from poor thermal stability and severe side reactions at temperatures above 60°C, failing to meet the practical use under high-temperature conditions. Here, we propose a high-temperature-resistant electrolyte system, i.e., high-boiling-point propylene carbonate, as well as dual-anion engineering to improve interface stability. The anion-regulated solvation structures achieve perfect compatibility between propylene carbonate and graphite, while the dual-anion synergy induces the formation of organic/inorganic gradient interphase dominated by C-F/LiB<i><sub>x</sub></i>O<i><sub>y</sub></i> species under high temperature. The LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> || graphite pouch cells demonstrate excellent cycling durability and rate capability under extreme conditions, achieving an outstanding lifespan of over 1000 cycles at 100°C, while retaining 55.7% of their rated capacity under a harsh 100°C and 5 C condition. Remarkably, the cells maintain normal electrochemical functionality even at 150°C, underscoring the robustness of the proposed electrolyte design.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"177 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129284","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In the past few years, a wide array of heterogeneous single-atom catalysts (SACs) has attracted researchers due to their exceptional performance in CO2 reduction. However, the role of defects in escalating the catalytic activity of SACs remains enigmatic. Through this review, we aim to provide a detailed understanding of the interplay between defects and catalytic activity in SACs. Despite remarkable advancements, a significant lacuna persists in fully elucidating the dynamic role of defects under operational conditions. This necessitates an integrated experimental and theoretical approach to guide the rational design of next-generation SACs for CO2 conversion. Therefore, we aim to account for mechanistic insights into SAC-led photochemical and electrochemical CO2 reduction reaction (CO2RR) without deviating from our objective of ascertaining the causes behind their catalytic efficiency due to defect engineering. The mechanistic toolkit derived from operando characterizations, density functional theory, and machine learning is provided to correlate defect-engineered SACs with improved activity and selectivity for CO2conversion.
{"title":"Synergizing Defect Chemistry and Single-Atom Catalysis: A Mechanistic Approach Toward Photochemical and Electrochemical CO2RR Applications","authors":"Syed Asim Ali, Iqra Sadiq, Tokeer Ahmad","doi":"10.1002/aenm.202506535","DOIUrl":"https://doi.org/10.1002/aenm.202506535","url":null,"abstract":"In the past few years, a wide array of heterogeneous single-atom catalysts (SACs) has attracted researchers due to their exceptional performance in CO<sub>2</sub> reduction. However, the role of defects in escalating the catalytic activity of SACs remains enigmatic. Through this review, we aim to provide a detailed understanding of the interplay between defects and catalytic activity in SACs. Despite remarkable advancements, a significant lacuna persists in fully elucidating the dynamic role of defects under operational conditions. This necessitates an integrated experimental and theoretical approach to guide the rational design of next-generation SACs for CO<sub>2</sub> conversion. Therefore, we aim to account for mechanistic insights into SAC-led photochemical and electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) without deviating from our objective of ascertaining the causes behind their catalytic efficiency due to defect engineering. The mechanistic toolkit derived from operando characterizations, density functional theory, and machine learning is provided to correlate defect-engineered SACs with improved activity and selectivity for CO<sub>2</sub>conversion.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"3 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129265","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jaeseong Kim, Incheol Heo, Dong-Kyung Kim, Min Seok Kang, Ji Hee Kwon, Byeong-Seon An, Keir C. Neuman, Byung-Hyun Kim, Hak-Sung Jung, Won Cheol Yoo
Lithium metal batteries (LMBs) offer exceptional energy density but are severely limited by dendrite formation and unstable interphases. Here, this work presents an electric field–driven in situ strategy to construct a vertically graded interphase using an oxygen-rich nanodiamond/carbon (O-ND/C) composite. During Li plating, conductive carbon migrates toward the current collector, forming a C-enriched conductive sublayer beneath a lithiophilic O-ND-rich insulating layer. This bilayer architecture homogenizes Li-ion flux, lowers the nucleation barrier, and simultaneously ensures mechanical robustness and electronic insulation, thereby enabling dendrite-free Li deposition. The optimized O-ND with 10 wt% of C interphase demonstrates outstanding electrochemical stability, maintaining an ultralow overpotential of 9.5 mV for 5800 h in symmetric cells and an average Coulombic efficiency (CE) of 98.8% to 700 cycles. In full-cell configurations with LiFePO4 cathodes, stable operation is sustained for up to 1500 cycles, areal capacity of 12.1 mAh cm−2 retained 9.9 mAh cm−2 after 50 cycles even under industrially relevant high cathode loading (93.8 mgLFP cm−2). Complementary density functional theory calculations confirm that O-ND surfaces enhance Li adsorption and diffusion, corroborating the experimental results. This work provides mechanistic insight into field-driven interphase engineering and offers a practical pathway toward safe, high-energy density LMBs.
{"title":"Electric-Field-Driven Bilayer Interphase from Oxygenated Nanodiamond-Carbon Nanoparticles for Dendrite-Free Lithium Metal Batteries","authors":"Jaeseong Kim, Incheol Heo, Dong-Kyung Kim, Min Seok Kang, Ji Hee Kwon, Byeong-Seon An, Keir C. Neuman, Byung-Hyun Kim, Hak-Sung Jung, Won Cheol Yoo","doi":"10.1002/aenm.202505964","DOIUrl":"https://doi.org/10.1002/aenm.202505964","url":null,"abstract":"Lithium metal batteries (LMBs) offer exceptional energy density but are severely limited by dendrite formation and unstable interphases. Here, this work presents an electric field–driven in situ strategy to construct a vertically graded interphase using an oxygen-rich nanodiamond/carbon (O-ND/C) composite. During Li plating, conductive carbon migrates toward the current collector, forming a C-enriched conductive sublayer beneath a lithiophilic O-ND-rich insulating layer. This bilayer architecture homogenizes Li-ion flux, lowers the nucleation barrier, and simultaneously ensures mechanical robustness and electronic insulation, thereby enabling dendrite-free Li deposition. The optimized O-ND with 10 wt% of C interphase demonstrates outstanding electrochemical stability, maintaining an ultralow overpotential of 9.5 mV for 5800 h in symmetric cells and an average Coulombic efficiency (CE) of 98.8% to 700 cycles. In full-cell configurations with LiFePO<sub>4</sub> cathodes, stable operation is sustained for up to 1500 cycles, areal capacity of 12.1 mAh cm<sup>−2</sup> retained 9.9 mAh cm<sup>−2</sup> after 50 cycles even under industrially relevant high cathode loading (93.8 mg<sub>LFP</sub> cm<sup>−2</sup>). Complementary density functional theory calculations confirm that O-ND surfaces enhance Li adsorption and diffusion, corroborating the experimental results. This work provides mechanistic insight into field-driven interphase engineering and offers a practical pathway toward safe, high-energy density LMBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"62 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sodium layered oxides NaxMO2 (x ≤ 1 and M = transition metal ions) have gained significant interest as sodium-ion battery (NIB) cathodes owing to their high operating voltages and potential for higher energy density compared with polyanion and Prussian blue–type cathodes. However, their practical applications are often hindered by the irreversible structural transitions leading to capacity fading during cycling. The nature and substitution of transition metal ions define the material properties and electrochemical performance. In this study, through comprehensive electrochemical characterization combined with multi-scale structural and spectroscopical analyses, we demonstrate the synergistic impacts of Lithium and Titanium doping, which not only increases overall capacity by boosting cation and anion cooperative redox contributions but also improves the rate capability and cycling stability. Specifically, Li+ doping enhances the available sodium inventory for extraction, while Ti4+ disrupts Na+/vacancy ordering at lower voltages (< 4 V) and mitigates the detrimental P2→OP4/O2 phase transition during cycling. The combined effect of Lithium and Titanium doping promotes more charge localization on Oxygen, which activates reversible lattice oxygen redox reactions at elevated voltages, contributing additional capacity beyond conventional cationic redox. This work provides crucial insights into the design of high-performance, high-capacity P2-type layered cathode materials for sodium-ion batteries.
{"title":"Engineering Na-Rich P2-Type Layered Oxides Through Li/Ti Dual Doping for Oxygen Redox Activation and Superior Structural Stability","authors":"Rishika Jakhar, Shrestha Ghosh, Adesh Rohan Mishra, Shristi Pradhan, Debalina Sarkar, Yuanlong Bill Zheng, Zengqing Zhuo, Tianyi Li, Lu Ma, Minghao Zhang, Shyue Ping Ong, Matthew Li, Leeann Sun, Prabhat Thapliyal, Jing Wang, Abhik Banerjee, Ying Shirley Meng","doi":"10.1002/aenm.202506119","DOIUrl":"https://doi.org/10.1002/aenm.202506119","url":null,"abstract":"Sodium layered oxides Na<i><sub>x</sub></i>MO<sub>2</sub> (<i>x</i> ≤ 1 and M = transition metal ions) have gained significant interest as sodium-ion battery (NIB) cathodes owing to their high operating voltages and potential for higher energy density compared with polyanion and Prussian blue–type cathodes. However, their practical applications are often hindered by the irreversible structural transitions leading to capacity fading during cycling. The nature and substitution of transition metal ions define the material properties and electrochemical performance. In this study, through comprehensive electrochemical characterization combined with multi-scale structural and spectroscopical analyses, we demonstrate the synergistic impacts of Lithium and Titanium doping, which not only increases overall capacity by boosting cation and anion cooperative redox contributions but also improves the rate capability and cycling stability. Specifically, Li<sup>+</sup> doping enhances the available sodium inventory for extraction, while Ti<sup>4</sup><sup>+</sup> disrupts Na<sup>+</sup>/vacancy ordering at lower voltages (< 4 V) and mitigates the detrimental P2→OP4/O2 phase transition during cycling. The combined effect of Lithium and Titanium doping promotes more charge localization on Oxygen, which activates reversible lattice oxygen redox reactions at elevated voltages, contributing additional capacity beyond conventional cationic redox. This work provides crucial insights into the design of high-performance, high-capacity P2-type layered cathode materials for sodium-ion batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"40 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146129266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Li Zhang, Jiawei Shi, Hansong Cheng, Fan Xia, Jing Li, Weiwei Cai, Ligang Feng
High-temperature proton exchange membrane fuel cells (HT-PEMFCs) suffer from severe performance degradation caused by phosphoric acid (PA) poisoning, which remains a critical challenge for practical applications. Unlike conventional techniques, herein, an electrostatic repulsion strategy is proposed to mitigate this issue by repelling the primary poisoning species (H2PO4−) away from Pt active sites through the construction of a local negative charge environment. To realize this concept, oxidized sulfur (SOx) groups are precisely incorporated into carbon support to generate localized negative electrostatics around Pt. Spectroscopic analyses and density functional theory calculations reveal strong Pt-support interactions that spatially enable electrostatic repulsion. As a result, the as-prepared Pt/C-SO catalyst exhibits high oxygen reduction reaction activity and outstanding durability in PA-containing electrolytes, far outperforming commercial Pt/C. When applied in HT-PEMFC, the Pt/C-SO catalyst delivers a maximum power density of 1166 mW cm−2 and maintains stable operation for over 500 h of continuous operation at 500 mA cm−2, with an ultra-low voltage decay rate of 26 µV h−1, which is nearly two orders of magnitude lower than that of commercial Pt/C (1075 µV h−1). This study provides a mechanistically grounded and practically feasible approach to overcoming PA poisoning and durability limitations of Pt-based catalysts in HT-PEMFCs.
{"title":"Electrostatic Repulsion Activates Durable Pt Catalysts for HT-PEMFCs","authors":"Li Zhang, Jiawei Shi, Hansong Cheng, Fan Xia, Jing Li, Weiwei Cai, Ligang Feng","doi":"10.1002/aenm.70724","DOIUrl":"https://doi.org/10.1002/aenm.70724","url":null,"abstract":"High-temperature proton exchange membrane fuel cells (HT-PEMFCs) suffer from severe performance degradation caused by phosphoric acid (PA) poisoning, which remains a critical challenge for practical applications. Unlike conventional techniques, herein, an electrostatic repulsion strategy is proposed to mitigate this issue by repelling the primary poisoning species (H<sub>2</sub>PO<sub>4</sub><sup>−</sup>) away from Pt active sites through the construction of a local negative charge environment. To realize this concept, oxidized sulfur (SO<sub>x</sub>) groups are precisely incorporated into carbon support to generate localized negative electrostatics around Pt. Spectroscopic analyses and density functional theory calculations reveal strong Pt-support interactions that spatially enable electrostatic repulsion. As a result, the as-prepared Pt/C-S<sub>O</sub> catalyst exhibits high oxygen reduction reaction activity and outstanding durability in PA-containing electrolytes, far outperforming commercial Pt/C. When applied in HT-PEMFC, the Pt/C-S<sub>O</sub> catalyst delivers a maximum power density of 1166 mW cm<sup>−2</sup> and maintains stable operation for over 500 h of continuous operation at 500 mA cm<sup>−2</sup>, with an ultra-low voltage decay rate of 26 µV h<sup>−1</sup>, which is nearly two orders of magnitude lower than that of commercial Pt/C (1075 µV h<sup>−1</sup>). This study provides a mechanistically grounded and practically feasible approach to overcoming PA poisoning and durability limitations of Pt-based catalysts in HT-PEMFCs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"9 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Nikhil Kalasariya, Paria Forozi Sowmeeh, Francisco Pena‐Camargo, Francesco Vanin, Tino Lukas, Yuxin Dong, Qifan Feng, Ziwei Liu, Waqar Ali Memon, Danpeng Gao, Jianqiu Gong, Xin Wu, Andres Felipe Castro Mendez, Jan Hagenberg, Zahra Abadi, Thomas Hultzsch, Xinyi Zhao, Sahil Shah, Hui Yu, Varun Srivastava, Jianbin Xu, Ni Zhao, Felix Lang, Zonglong Zhu, Martin Stolterfoht
Halide segregation (HS) is considered to be one of the most significant hurdles for the commercialization of tandem solar cells. However, despite significant research on this matter, the exact impact of HS on the performance degradation and the ion density evolution is yet to be established. In this work, we investigate the intriguing correlation between HS, ion‐induced efficiency losses, and ion density evolution in wide‐bandgap (WBG) triple cation perovskite cells. Our results highlight that all three phenomena evolve on similar timescales and follow the same trend across all studied bandgaps. This implies that the poor energy‐lifetime product observed for devices prone to halide segregation is a result of enhanced ionic losses rather than, for instance, charge carrier funneling. Furthermore, reminiscent of the recovery of HS observed previously, we demonstrate that ionic losses also recover after light exposure and dark storage, which occurs along with a receding ion density. However, we also observe irreversible ionic losses, especially after prolonged illumination, which are critical for device operation. These findings present an important new understanding of the interplay between halide segregation and ionic processes and provide a rational explanation for the performance and stability of mixed halide WBG perovskites.
{"title":"How Halide Segregation Governs the Ion Density Evolution and Ionic Performance Losses: From Degradation to Recovery","authors":"Nikhil Kalasariya, Paria Forozi Sowmeeh, Francisco Pena‐Camargo, Francesco Vanin, Tino Lukas, Yuxin Dong, Qifan Feng, Ziwei Liu, Waqar Ali Memon, Danpeng Gao, Jianqiu Gong, Xin Wu, Andres Felipe Castro Mendez, Jan Hagenberg, Zahra Abadi, Thomas Hultzsch, Xinyi Zhao, Sahil Shah, Hui Yu, Varun Srivastava, Jianbin Xu, Ni Zhao, Felix Lang, Zonglong Zhu, Martin Stolterfoht","doi":"10.1002/aenm.202503866","DOIUrl":"https://doi.org/10.1002/aenm.202503866","url":null,"abstract":"Halide segregation (HS) is considered to be one of the most significant hurdles for the commercialization of tandem solar cells. However, despite significant research on this matter, the exact impact of HS on the performance degradation and the ion density evolution is yet to be established. In this work, we investigate the intriguing correlation between HS, ion‐induced efficiency losses, and ion density evolution in wide‐bandgap (WBG) triple cation perovskite cells. Our results highlight that all three phenomena evolve on similar timescales and follow the same trend across all studied bandgaps. This implies that the poor energy‐lifetime product observed for devices prone to halide segregation is a result of enhanced ionic losses rather than, for instance, charge carrier funneling. Furthermore, reminiscent of the recovery of HS observed previously, we demonstrate that ionic losses also recover after light exposure and dark storage, which occurs along with a receding ion density. However, we also observe irreversible ionic losses, especially after prolonged illumination, which are critical for device operation. These findings present an important new understanding of the interplay between halide segregation and ionic processes and provide a rational explanation for the performance and stability of mixed halide WBG perovskites.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122286","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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