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Compositional Tuning and Surface Restructuring Synergistically Enhance Perovskite Ferrite Catalysts for Hydrogen Evolution in a Membrane-Less Electrolyzer 无膜电解槽中钙钛矿铁氧体析氢催化剂的成分调整和表面重组协同增强
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-08 DOI: 10.1002/aenm.202505486
Yixin Bi, Yuhao Wang, Zilong Wang, Yufei Song, Nuotong Li, Jingwei Li, Arini Kar, Qing Chen, Francesco Ciucci
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。
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引用次数: 0
Streamlined Y6-Analogs Enabling Efficient Ambient-Air-Processed Organic Solar Cells 流线型y6类似物实现高效的环境空气处理有机太阳能电池
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-08 DOI: 10.1002/aenm.202505110
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。
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引用次数: 0
Multiscale Interfacial Regulation for Stable Zinc Anodes: From Fundamental Mechanisms to Practical Applications 稳定锌阳极的多尺度界面调控:从基本机制到实际应用
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-08 DOI: 10.1002/aenm.70704
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.
水锌离子电池(AZIBs)由于其固有的安全性和低成本而成为大规模储能的有希望的候选者。然而,它们的商业化受到臭名昭著的锌阳极问题的阻碍,包括不受控制的枝晶生长和寄生副反应。最近,多尺度界面调节作为应对这些挑战的变革性策略出现了。该方法通过构建多层结构和优化界面耦合,克服了单界面调制的局限性,从而提供了有效的阳极保护。为了促进锌的均匀电镀和抑制副反应,本文综述了跨多物理场优化、锌沉积方向优化和电解质溶剂化结构优化的多尺度策略。我们系统地介绍了将这些多尺度策略应用于锌箔、锌粉和基于主体的阳极,以及分离器和水凝胶电解质方面的最新进展,重点介绍了它们的设计原则、潜在机制和特定场景的适用性。此外,我们阐明了该技术如何通过功能互补的多层、双面或梯度界面实现离子传输、沉积行为和界面环境的协同优化,从而系统地减轻锌阳极失效。最后,讨论了未来的研究方向和挑战,强调深刻的机理理解加上合理的设计对于释放下一代azib的全部潜力至关重要。
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引用次数: 0
Functionalized and Customized Electrolyte Enabling NCM811||Gr Pouch Cells Operation at 150°C 功能化和定制的电解质使NCM811||Gr袋状电池在150°C下工作
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1002/aenm.70718
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.
随着锂离子电池应用的不断扩大,对高性能耐高温锂离子电池的需求日益增长,特别是在军事或航空航天探索等领域。然而,传统电解质在60℃以上的温度下热稳定性差,副反应严重,无法满足高温条件下的实际使用。在这里,我们提出了一种耐高温的电解质体系,即高沸点碳酸丙烯酯,以及双阴离子工程来提高界面稳定性。阴离子调节的溶剂化结构实现了碳酸丙烯酯与石墨的完美相容性,双阴离子协同作用在高温下形成以C-F/LiBxOy物质为主的有机/无机梯度界面相。LiNi0.8Co0.1Mn0.1O2 ||石墨袋电池在极端条件下表现出出色的循环耐久性和倍率能力,在100°C下实现了超过1000次循环的出色寿命,同时在恶劣的100°C和5°C条件下保持了55.7%的额定容量。值得注意的是,即使在150°C下,电池也能保持正常的电化学功能,这强调了所提出的电解质设计的稳健性。
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引用次数: 0
Synergizing Defect Chemistry and Single-Atom Catalysis: A Mechanistic Approach Toward Photochemical and Electrochemical CO2RR Applications 协同缺陷化学和单原子催化:光化学和电化学CO2RR应用的机理途径
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1002/aenm.202506535
Syed Asim Ali, Iqra Sadiq, Tokeer Ahmad
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.
在过去的几年里,各种各样的非均相单原子催化剂(SACs)因其在二氧化碳还原方面的优异性能而吸引了研究人员的注意。然而,缺陷在提高SACs催化活性中的作用仍然是一个谜。通过这篇综述,我们的目的是提供一个详细的了解在sac缺陷和催化活性之间的相互作用。尽管取得了显著的进步,但在充分阐明运行条件下缺陷的动态作用方面仍然存在显著的空白。这就需要一个综合的实验和理论方法来指导下一代二氧化碳转换sac的合理设计。因此,我们的目标是在不偏离我们确定其催化效率背后的原因的情况下,解释sac主导的光化学和电化学CO2还原反应(CO2RR)的机制见解。从operando特征、密度泛函理论和机器学习中衍生出来的机械工具包,可以将缺陷工程sac与改进的co2转换活性和选择性联系起来。
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引用次数: 0
Electric-Field-Driven Bilayer Interphase from Oxygenated Nanodiamond-Carbon Nanoparticles for Dendrite-Free Lithium Metal Batteries 无枝晶锂金属电池用氧化纳米金刚石-碳纳米颗粒的电场驱动双层界面
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1002/aenm.202505964
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}
引用次数: 0
Engineering Na-Rich P2-Type Layered Oxides Through Li/Ti Dual Doping for Oxygen Redox Activation and Superior Structural Stability Li/Ti双掺杂工程富钠p2型层状氧化物的氧氧化还原活化和优异的结构稳定性
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1002/aenm.202506119
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
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.
与聚阴离子和普鲁士蓝阴极相比,钠层状氧化物NaxMO2 (x≤1和M =过渡金属离子)具有较高的工作电压和更高的能量密度,因此作为钠离子电池(NIB)阴极获得了极大的兴趣。然而,它们的实际应用往往受到循环过程中不可逆的结构转变导致容量衰减的阻碍。过渡金属离子的性质和取代决定了材料的性质和电化学性能。在本研究中,通过综合电化学表征结合多尺度结构和光谱分析,我们证明了锂和钛掺杂的协同效应,不仅通过促进阳离子和阴离子的协同氧化还原贡献来提高总容量,而且还提高了速率能力和循环稳定性。具体来说,Li+掺杂增加了可用于提取的钠库存,而Ti4+在较低电压(< 4v)下破坏Na+/空位有序,并减轻了循环过程中有害的P2→OP4/O2相变。锂和钛掺杂的共同作用促进了氧上更多的电荷定位,在高电压下激活可逆的晶格氧氧化还原反应,提供了比传统阳离子氧化还原更大的容量。这项工作为设计用于钠离子电池的高性能、高容量p2型层状正极材料提供了重要的见解。
{"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 (&lt; 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}
引用次数: 0
Electrostatic Repulsion Activates Durable Pt Catalysts for HT-PEMFCs 静电斥力激活ht - pemfc的耐用Pt催化剂
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-06 DOI: 10.1002/aenm.70724
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。
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引用次数: 0
How Halide Segregation Governs the Ion Density Evolution and Ionic Performance Losses: From Degradation to Recovery 卤化物偏析如何控制离子密度演变和离子性能损失:从降解到恢复
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-05 DOI: 10.1002/aenm.202503866
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.
卤化物分离(HS)被认为是串联太阳能电池商业化的最大障碍之一。然而,尽管对这一问题进行了大量研究,但HS对性能下降和离子密度演变的确切影响尚未确定。在这项工作中,我们研究了宽带隙(WBG)三阳离子钙钛矿电池中HS、离子诱导效率损失和离子密度演变之间的有趣相关性。我们的研究结果强调,这三种现象在相似的时间尺度上演变,并在所有研究的带隙中遵循相同的趋势。这意味着,对于易于发生卤化物偏析的器件,观察到的较差的能量寿命产物是离子损失增强的结果,而不是电荷载流子漏斗的结果。此外,与之前观察到的HS恢复类似,我们证明了离子损失在光暴露和暗储存后也会恢复,这伴随着离子密度的下降而发生。然而,我们也观察到不可逆的离子损失,特别是在长时间照明后,这对设备操作至关重要。这些发现为卤化物偏析与离子过程之间的相互作用提供了重要的新认识,并为混合卤化物WBG钙钛矿的性能和稳定性提供了合理的解释。
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引用次数: 0
Effects of Mechanical Properties of Elastomeric Electrolytes for Stable Operation of Lithium Metal Batteries (Adv. Energy Mater. 5/2026) 弹性电解质力学性能对锂金属电池稳定运行的影响(能源材料,5/2026)
IF 27.8 1区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-04 DOI: 10.1002/aenm.70512
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}
引用次数: 0
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