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.
平衡析氢反应电催化的稳定性和活性对先进的电解技术来说仍然是一个挑战。这项工作引入了一种协同设计策略，以应对现场表面重构的挑战。铁基双钙钛矿具有最优的HER催化电子结构，在0.1 m KOH和1 m KOH下，在10 mA/cm2下的过电位分别为325 mV和184 mV，是目前报道的最好的。此外，该催化剂表现出显著的自改善稳定性，在300 mV过电位作用20 h后，其比活性提高了1.98倍，这是由于透射电镜证实了非晶层的重组。为了证明其实用性，该催化剂被集成到一个活性流动无膜电解槽（AFME）中，这是一项很有前途的技术，但目前受到不稳定性的限制。该装置在50 mA/cm2下表现出1000小时的出色运行稳定性，最小衰减率为0.25 mV/h，为无膜系统建立了新的基准。这项工作不仅为设计自我改进的催化剂提供了强有力的策略，而且验证了其在下一代电解槽技术中的实际功效，为经济高效的绿色制氢铺平了道路。
{"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.
在环境加工条件下实现高效率和长期稳定性仍然是有机太阳能电池（OSCs）商业化的关键障碍。在这里，我们报道了两种新的y6类似物——BT(BO)-v-T(C12)-4F （4F）和BT(BO)-v-T(C12)-4Cl （4Cl）——具有乙烯(v)桥接DA - d核心，旨在提高材料的可扩展性，同时保持y6型受体的结构优势。形态学和器件级研究表明，即使在空气中完全加工，这些M-Y6衍生物也能促进热力学稳定的分子包装和有利的晶体取向。通过可重复的空气处理协议，将4F与D18/L8-BO逐层三元结构结合，可获得19%的认证功率转换效率（PCE），是在环境条件下制造的传统OSCs中最高的。此外，基于4f的器件表现出优异的热稳定性和光稳定性，在iso - l -1协议下延长老化后，在没有封装的情况下保留了80%以上的初始PCE。这些改进归功于4F受体增强的结晶度、垂直分子排列和形态稳健性。本研究确定BT(BO)-v-T(C12)-4F是一种很有前途的空气处理受体，可用于可扩展的OSCs，兼具高效率和长期运行耐久性。
{"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.
锂金属电池（lmb）具有优异的能量密度，但受到枝晶形成和界面不稳定的严重限制。在这里，这项工作提出了一种电场驱动的原位策略，使用富氧纳米金刚石/碳（O-ND/C）复合材料构建垂直梯度界面。在镀锂过程中，导电碳向集热器迁移，在亲锂的富o - nd绝缘层下形成富c导电亚层。这种双层结构使锂离子通量均匀化，降低了成核屏障，同时保证了机械稳健性和电子绝缘性，从而实现了无枝晶的锂沉积。优化后的O-ND具有优异的电化学稳定性，在对称电池中保持9.5 mV的超低过电位5800 h，平均库仑效率（CE）为98.8%至700次循环。在使用LiFePO4阴极的全电池配置中，稳定运行长达1500次循环，即使在工业相关的高阴极负载（93.8 mgLFP cm - 2）下，循环50次后，12.1 mAh cm - 2的面容量仍保持9.9 mAh cm - 2。互补密度泛函理论计算证实了O-ND表面增强了Li的吸附和扩散，证实了实验结果。这项工作为现场驱动的相间工程提供了机理见解，并为实现安全、高能量密度的lmb提供了切实可行的途径。
{"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.
高温质子交换膜燃料电池（ht - pemfc）在磷酸（PA）中毒的情况下性能会严重下降，这是其在实际应用中面临的一个严峻挑战。与传统技术不同，本文提出了一种静电斥力策略，通过构建局部负电荷环境，将主要中毒物质（H2PO4−）从Pt活性位点赶走，从而缓解了这一问题。为了实现这一概念，氧化硫（SOx）基团被精确地整合到碳载体中，以在铂周围产生局部的负静电。光谱分析和密度泛函理论计算表明，Pt-载体之间的强相互作用在空间上使静电排斥成为可能。结果表明，制备的Pt/C- so催化剂在含pa电解质中表现出较高的氧还原反应活性和优异的耐久性，远远优于商业Pt/C。当应用于HT-PEMFC时，Pt/C- so催化剂提供了1166 mW cm - 2的最大功率密度，并在500 mA cm - 2下连续运行超过500小时，具有26 μ V h - 1的超低电压衰减率，比商用Pt/C （1075 μ V h - 1）低近两个数量级。该研究为克服ht - pemfc中PA中毒和pt基催化剂的耐久性限制提供了一种机制基础和实际可行的方法。
{"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}
Dongkyu Lee, Dongguk Kang, Chanho Yuk, Hyeri Kang, Eunji Lee, Wonho Lee, Jinseok Park, Bumjoon J. Kim
{"title":"Effects of Mechanical Properties of Elastomeric Electrolytes for Stable Operation of Lithium Metal Batteries (Adv. Energy Mater. 5/2026)","authors":"Dongkyu Lee, Dongguk Kang, Chanho Yuk, Hyeri Kang, Eunji Lee, Wonho Lee, Jinseok Park, Bumjoon J. Kim","doi":"10.1002/aenm.70512","DOIUrl":"https://doi.org/10.1002/aenm.70512","url":null,"abstract":"","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"89 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122287","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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