Sun‐Ju Kim, Seungyeon Hong, Dong‐Geon Kwun, Yu Jin Kang, Thanh‐Danh Nguyen, In Hwa Cho, Sung Hun Lee, Gyeong‐Cheon Choi, Geun‐young Yoon, Siyeon Seo, Weifan Luo, Ghewa Alsabeh, Dong‐Hwan Hwang, Min Jun Choi, Jong‐Min Kim, Olzhas Kurman, Dong‐Ok Kim, Sohyun Park, Jong H. Kim, O‐Pil Kwon, Jovana V. Milić, Michael Grätzel, Do‐Hyung Kim, Hyo Jung Kim, Ji‐Youn Seo
Scaling high‐efficiency perovskite solar cells into commercially viable modules remains challenging. Here, we demonstrate a seed‐primed, vacuum‐assisted crystallization (S‐VAC) strategy that links oleylamine‐induced α‐phase nanocrystal seeding to vacuum‐driven vertical crystal growth. Complementary in situ characterization, including time‐resolved GIWAXS, solution‐state NMR, and dynamic light scattering (DLS), reveals that oleylamine forms uniform ≈1.7 nm α‐phase seeds in the precursor solution via hydrogen bonding with FA + cations and steric stabilization. These seeds prime the substrate for controlled, single‐crystal‐like vertical growth under low‐pressure vacuum processing, thereby eliminating the need for toxic antisolvents. The resulting monolithic perovskite films exhibit strong (100) texture and high uniformity across 15 × 15 cm 2 substrates. Using S‐VAC, we achieve a power conversion efficiency (PCE) of 23.2% for 2.5 × 2.5 cm 2 devices and a certified efficiency of 19.1% for 15 × 15 cm 2 mini‐modules. Encapsulated modules retain >94% of their initial efficiency after one year of continuous outdoor operation. By establishing a molecular‐level basis for oleylamine‐assisted seed formation and demonstrating scalable, antisolvent‐free processing, this work advances seed‐assisted crystallization and supports the practical commercialization of robust and sustainable perovskite photovoltaics.
将高效钙钛矿太阳能电池扩展到商业上可行的组件仍然具有挑战性。在这里，我们展示了一种种子启动，真空辅助结晶（S - VAC）策略，将油胺诱导的α相纳米晶体播种与真空驱动的垂直晶体生长联系起来。互补的原位表征，包括时间分辨GIWAXS，溶液态NMR和动态光散射（DLS），揭示了油胺通过与FA +阳离子的氢键和空间稳定在前驱体溶液中形成均匀的≈1.7 nm α相种子。这些种子为在低压真空处理下可控的单晶类垂直生长的底物提供基质，从而消除了对有毒抗溶剂的需求。所得到的单片钙钛矿薄膜在15 × 15 cm 2的衬底上表现出强烈的（100）纹理和高均匀性。使用S - VAC，我们在2.5 × 2.5 cm 2器件上实现了23.2%的功率转换效率（PCE），在15 × 15 cm 2微型模块上实现了19.1%的认证效率。封装模块在室外连续运行一年后仍能保持其初始效率的94%。通过建立一个分子水平的胺辅助种子形成的基础，并展示了可扩展的，无抗溶剂的处理，这项工作推进了种子辅助结晶，并支持了强大和可持续的钙钛矿光伏的实际商业化。
{"title":"Uniform Monolithic Perovskite Films for Scalable Modules: Anti‐Solvent‐Free Crystallization via Seed Priming and Vacuum Processing","authors":"Sun‐Ju Kim, Seungyeon Hong, Dong‐Geon Kwun, Yu Jin Kang, Thanh‐Danh Nguyen, In Hwa Cho, Sung Hun Lee, Gyeong‐Cheon Choi, Geun‐young Yoon, Siyeon Seo, Weifan Luo, Ghewa Alsabeh, Dong‐Hwan Hwang, Min Jun Choi, Jong‐Min Kim, Olzhas Kurman, Dong‐Ok Kim, Sohyun Park, Jong H. Kim, O‐Pil Kwon, Jovana V. Milić, Michael Grätzel, Do‐Hyung Kim, Hyo Jung Kim, Ji‐Youn Seo","doi":"10.1002/aenm.202506521","DOIUrl":"https://doi.org/10.1002/aenm.202506521","url":null,"abstract":"Scaling high‐efficiency perovskite solar cells into commercially viable modules remains challenging. Here, we demonstrate a seed‐primed, vacuum‐assisted crystallization (S‐VAC) strategy that links oleylamine‐induced α‐phase nanocrystal seeding to vacuum‐driven vertical crystal growth. Complementary in situ characterization, including time‐resolved GIWAXS, solution‐state NMR, and dynamic light scattering (DLS), reveals that oleylamine forms uniform ≈1.7 nm α‐phase seeds in the precursor solution via hydrogen bonding with FA <jats:sup>+</jats:sup> cations and steric stabilization. These seeds prime the substrate for controlled, single‐crystal‐like vertical growth under low‐pressure vacuum processing, thereby eliminating the need for toxic antisolvents. The resulting monolithic perovskite films exhibit strong (100) texture and high uniformity across 15 × 15 cm <jats:sup>2</jats:sup> substrates. Using S‐VAC, we achieve a power conversion efficiency (PCE) of 23.2% for 2.5 × 2.5 cm <jats:sup>2</jats:sup> devices and a certified efficiency of 19.1% for 15 × 15 cm <jats:sup>2</jats:sup> mini‐modules. Encapsulated modules retain >94% of their initial efficiency after one year of continuous outdoor operation. By establishing a molecular‐level basis for oleylamine‐assisted seed formation and demonstrating scalable, antisolvent‐free processing, this work advances seed‐assisted crystallization and supports the practical commercialization of robust and sustainable perovskite photovoltaics.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"41 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146033826","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}
Hadi Heidary, Vahid Nasrollahi, Daniel Wilmot, Jacob Bracegirdle‐Morais, Sophie C. Cox, Stefan Dimov, Moataz M. Attallah, Ahmad El‐kharouf, Sara Walker, Robert Steinberger‐Wilckens
The integration of hydrogen fuel cells into aerospace applications is limited by the weight and volume of fuel cell systems. Currently, bipolar plates account for 80 % of fuel cell stack mass and 60 % of its volume. Herein, we leverage a range of advanced manufacturing techniques to develop novel lightweight‐compact porous distributors with ultrahigh power densities. Research begins with a graphene‐coated nickel foam porous distributor, which enhances reactants transport and interfacial conductivity, achieving a power density of 1.52 W/cm 2 , ∼50 % improvement over conventional designs. To further boost gravimetric power density, titanium was adopted as a base material, and porous architectures were optimized using Computational Fluid Dynamics to ensure optimal reactant distribution and water management. To realize these porous titanium designs, two advanced manufacturing techniques were leveraged: laser powder bed fusion (LPBF) and laser micromachining. While the optimized LPBF lattice structure reached 1.36 W/cm 2 , the laser‐patterned non‐homogeneous architecture demonstrated a breakthrough performance of 1.62 W/cm 2 , translating to volumetric and gravimetric power densities of over 10 kW/L and 9 kW/kg, respectively. These values surpass current commercial benchmarks and exceed EU/UK 2030 targets. We demonstrate how integrating digital design, flow control, advanced materials, and manufacturing enables lightweight, high‐power fuel cells, with broader impact on electrolyzers, heat exchangers, and batteries.
{"title":"Leveraging Digital Advanced Manufacturing to Enable Polymer Electrolyte Fuel Cells With Ultrahigh Gravimetric Power Density","authors":"Hadi Heidary, Vahid Nasrollahi, Daniel Wilmot, Jacob Bracegirdle‐Morais, Sophie C. Cox, Stefan Dimov, Moataz M. Attallah, Ahmad El‐kharouf, Sara Walker, Robert Steinberger‐Wilckens","doi":"10.1002/aenm.202504454","DOIUrl":"https://doi.org/10.1002/aenm.202504454","url":null,"abstract":"The integration of hydrogen fuel cells into aerospace applications is limited by the weight and volume of fuel cell systems. Currently, bipolar plates account for 80 % of fuel cell stack mass and 60 % of its volume. Herein, we leverage a range of advanced manufacturing techniques to develop novel lightweight‐compact porous distributors with ultrahigh power densities. Research begins with a graphene‐coated nickel foam porous distributor, which enhances reactants transport and interfacial conductivity, achieving a power density of 1.52 W/cm <jats:sup>2</jats:sup> , ∼50 % improvement over conventional designs. To further boost gravimetric power density, titanium was adopted as a base material, and porous architectures were optimized using Computational Fluid Dynamics to ensure optimal reactant distribution and water management. To realize these porous titanium designs, two advanced manufacturing techniques were leveraged: laser powder bed fusion (LPBF) and laser micromachining. While the optimized LPBF lattice structure reached 1.36 W/cm <jats:sup>2</jats:sup> , the laser‐patterned non‐homogeneous architecture demonstrated a breakthrough performance of 1.62 W/cm <jats:sup>2</jats:sup> , translating to volumetric and gravimetric power densities of over 10 kW/L and 9 kW/kg, respectively. These values surpass current commercial benchmarks and exceed EU/UK 2030 targets. We demonstrate how integrating digital design, flow control, advanced materials, and manufacturing enables lightweight, high‐power fuel cells, with broader impact on electrolyzers, heat exchangers, and batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"7 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146033828","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}
Lithium-rich manganese-based layered oxides (LRMOs) are leading candidates for next-generation high-energy-density lithium-ion batteries, offering exceptional specific capacities exceeding 250 mAh g−1. However, interfacial instability and surface structural degradation impede their commercial deployment. Current research lacks comprehensive analysis of dynamic interfacial mechanisms governing oxygen redox and corresponding engineering strategies. This review focuses on recent advancements in interface engineering to enhance the reversibility of anionic redox reactions in LRMOs, providing crucial insights for designing high-performance batteries. The LRMO crystal structure, oxygen redox mechanism, and associated challenges are first outlined. Subsequently, we examine interfacial design progress including surface engineering, surface defect regulation, integrated modifications, and electrolyte engineering, highlighting how these approaches improve oxygen redox reversibility to mitigate the performance decline of LRMOs. Additionally, the mechanical and chemical instability mechanisms of all-solid-state battery interfaces and corresponding interface design strategies are discussed. Finally, we provide further insights and new perspectives for the better development of LRMO cathode materials.
富锂锰基层状氧化物（LRMOs）是下一代高能量密度锂离子电池的主要候选材料，具有超过250 mAh g−1的特殊容量。然而，界面不稳定和表面结构退化阻碍了它们的商业应用。目前的研究缺乏对控制氧氧化还原的动态界面机制的全面分析和相应的工程策略。本文综述了界面工程的最新进展，以增强LRMOs中阴离子氧化还原反应的可逆性，为设计高性能电池提供重要见解。首先概述了LRMO的晶体结构、氧氧化还原机理和相关挑战。随后，我们研究了界面设计的进展，包括表面工程、表面缺陷调节、集成修饰和电解质工程，重点介绍了这些方法如何提高氧氧化还原可逆性，以减轻LRMOs的性能下降。此外，还讨论了全固态电池界面的力学和化学不稳定性机制以及相应的界面设计策略。最后，对LRMO正极材料的进一步发展提出了新的见解和展望。
{"title":"Interface Engineering for Heightening Anionic Redox Reversibility of Li-Rich Layered Oxides Cathodes: Recent Advances and Perspectives","authors":"Yuhang Lou, Hai Yang, Yan Yu","doi":"10.1002/aenm.202506755","DOIUrl":"https://doi.org/10.1002/aenm.202506755","url":null,"abstract":"Lithium-rich manganese-based layered oxides (LRMOs) are leading candidates for next-generation high-energy-density lithium-ion batteries, offering exceptional specific capacities exceeding 250 mAh g<sup>−1</sup>. However, interfacial instability and surface structural degradation impede their commercial deployment. Current research lacks comprehensive analysis of dynamic interfacial mechanisms governing oxygen redox and corresponding engineering strategies. This review focuses on recent advancements in interface engineering to enhance the reversibility of anionic redox reactions in LRMOs, providing crucial insights for designing high-performance batteries. The LRMO crystal structure, oxygen redox mechanism, and associated challenges are first outlined. Subsequently, we examine interfacial design progress including surface engineering, surface defect regulation, integrated modifications, and electrolyte engineering, highlighting how these approaches improve oxygen redox reversibility to mitigate the performance decline of LRMOs. Additionally, the mechanical and chemical instability mechanisms of all-solid-state battery interfaces and corresponding interface design strategies are discussed. Finally, we provide further insights and new perspectives for the better development of LRMO cathode materials.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"43 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022026","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}
Reducing the precious Pt loading in catalyst layers (CLs) while maintaining fuel cell performance is critical for cost reduction, necessitating the development of an optimized CL microstructure, but conventional empirical expertise‐dependent trial‐and‐error optimization faces severe efficiency limitations when dealing with multiple transfers coupled with electrochemical reactions inside the multi‐component hierarchical porous architecture. Here, we present Generative Artificial Intelligence for Controllable Electrode Synthesis (GAI4CES), a framework that enables rapid CL microstructure synthesis, achieving nearly 500x speedup for constructing a representative CL microstructure of 128 nm 3 (in 0.36 s compared to 168 s required by traditional numerical methods). It can tailor key property constraints, such as Pt loading and electrochemical surface area (ECSA), to generate statistically representative microstructures satisfying target specifications. This capability enables an exhaustive search for the optimal CL structural design through large‐scale geometry‑constrained synthesis coupled with fast performance prediction. The optimized CL microstructure achieves an improvement of 11.6% in ECSA and a reduction of 32.9% in average ionomer thickness surrounding the Pt/C at ultralow Pt loading (e.g., 0.05 mg cm −2 ), and contributes to a maximum 70.2% voltage increase at 3 A cm −2 , indicating that the GAI4CES is powerful in promoting the development of advanced low‐cost and high‐performance fuel cells.
在保持燃料电池性能的同时，减少催化剂层（CL）中宝贵的铂负载对于降低成本至关重要，因此需要开发优化的CL微观结构，但是，当处理多组分分层多孔结构内的多重转移和电化学反应时，传统的依赖经验专业知识的试错优化面临严重的效率限制。在这里，我们提出了用于可控电极合成的生成式人工智能（GAI4CES），这是一个能够快速合成CL微观结构的框架，在构建128 nm 3的代表性CL微观结构时实现了近500倍的加速（与传统数值方法所需的168 s相比，耗时0.36 s）。它可以定制关键性能约束，如Pt负载和电化学表面积（ECSA），以生成满足目标规格的统计代表性微结构。这种能力可以通过大规模几何约束合成以及快速性能预测来实现对最佳CL结构设计的详尽搜索。优化后的CL微结构在超低Pt负载（例如0.05 mg cm - 2）下的ECSA提高了11.6%，Pt/C周围的平均离子厚度减少了32.9%，并且在3 a cm - 2时最大电压提高了70.2%，这表明GAI4CES在促进先进低成本高性能燃料电池的发展方面具有强大的作用。
{"title":"Deep Generative Models Regulate Ultralow‐Pt Catalyst Layer in Fuel Cells","authors":"Qiang Zheng, Yutong Mu, Guobin Zhang, Xingyi Shi, Dongxiao Zhang","doi":"10.1002/aenm.202506271","DOIUrl":"https://doi.org/10.1002/aenm.202506271","url":null,"abstract":"Reducing the precious Pt loading in catalyst layers (CLs) while maintaining fuel cell performance is critical for cost reduction, necessitating the development of an optimized CL microstructure, but conventional empirical expertise‐dependent trial‐and‐error optimization faces severe efficiency limitations when dealing with multiple transfers coupled with electrochemical reactions inside the multi‐component hierarchical porous architecture. Here, we present Generative Artificial Intelligence for Controllable Electrode Synthesis (GAI4CES), a framework that enables rapid CL microstructure synthesis, achieving nearly 500x speedup for constructing a representative CL microstructure of 128 nm <jats:sup>3</jats:sup> (in 0.36 s compared to 168 s required by traditional numerical methods). It can tailor key property constraints, such as Pt loading and electrochemical surface area (ECSA), to generate statistically representative microstructures satisfying target specifications. This capability enables an exhaustive search for the optimal CL structural design through large‐scale geometry‑constrained synthesis coupled with fast performance prediction. The optimized CL microstructure achieves an improvement of 11.6% in ECSA and a reduction of 32.9% in average ionomer thickness surrounding the Pt/C at ultralow Pt loading (e.g., 0.05 mg cm <jats:sup>−</jats:sup> <jats:sup>2</jats:sup> ), and contributes to a maximum 70.2% voltage increase at 3 A cm <jats:sup>−</jats:sup> <jats:sup>2</jats:sup> , indicating that the GAI4CES is powerful in promoting the development of advanced low‐cost and high‐performance fuel cells.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"261 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146033827","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}
Featuring unique selective absorption, the semi‐transparent organic photovoltaics (ST‐OPVs) hold a bright future for building integration. However, the prevailing ST‐OPVs take a transmission mode (t‐ST‐OPV) and can hardly achieve a good compromise between the averaged visible transmission (AVT) and power conversion efficiency (PCE), rendering a poor light utilization efficiency (LUE) and limiting their practical application. Inspired by the optical path of a periscope, this work developed an ST‐OPV structure with a reflection optical path (r‐ST‐OPV), which takes dual or multiple reflections to make a transmission effect. This structure mitigates the reflection loss and significantly enhances the absorbing selectivity. Facilitated by the sophisticated optical manipulation technique, the r‐ST‐OPV with almost full invisible transmission (AVT ∼ 92.2%) and a PCE of 8.27% is achieved, corresponding to a record LUE of 7.62% among all ST‐OPVs. This work opens up the avenue toward high‐performance organic solar windows for practical application.
半透明有机光伏材料（ST - opv）具有独特的选择性吸收特性，在建筑集成领域具有广阔的应用前景。然而，目前流行的ST - OPV采用一种传输模式（t - ST - OPV），很难在平均可见光透射率（AVT）和功率转换效率（PCE）之间取得很好的折衷，导致光利用效率（LUE）较差，限制了它们的实际应用。受潜望镜光路的启发，本研究开发了一种具有反射光路（r - ST - OPV）的ST - OPV结构，该结构需要双重或多次反射才能产生传输效果。这种结构减轻了反射损失，显著提高了吸收选择性。在复杂的光学操作技术的帮助下，r‐ST‐OPV实现了几乎完全不可见透射（AVT ~ 92.2%）和8.27%的PCE，对应于所有ST‐OPV中创纪录的7.62%的LUE。这项工作为实际应用的高性能有机太阳能窗开辟了道路。
{"title":"Periscope‐Inspired High‐Performance Semitransparent Organic Photovoltaics With Dual Surface‐Reflection Optical Structure","authors":"Yiming Wang, Xiangjun Zheng, Jingde Chen, Yuqian Tian, Yaokai Li, Tianyi Chen, Mengting Wang, Xiaoling Wu, Jianxin Tang, Qiang Li, Hongzheng Chen, Lijian Zuo","doi":"10.1002/aenm.202505427","DOIUrl":"https://doi.org/10.1002/aenm.202505427","url":null,"abstract":"Featuring unique selective absorption, the semi‐transparent organic photovoltaics (ST‐OPVs) hold a bright future for building integration. However, the prevailing ST‐OPVs take a transmission mode (t‐ST‐OPV) and can hardly achieve a good compromise between the averaged visible transmission (AVT) and power conversion efficiency (PCE), rendering a poor light utilization efficiency (LUE) and limiting their practical application. Inspired by the optical path of a periscope, this work developed an ST‐OPV structure with a reflection optical path (r‐ST‐OPV), which takes dual or multiple reflections to make a transmission effect. This structure mitigates the reflection loss and significantly enhances the absorbing selectivity. Facilitated by the sophisticated optical manipulation technique, the r‐ST‐OPV with almost full invisible transmission (AVT ∼ 92.2%) and a PCE of 8.27% is achieved, corresponding to a record LUE of 7.62% among all ST‐OPVs. This work opens up the avenue toward high‐performance organic solar windows for practical application.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"39 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146033829","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}
Jingxiu Wang, Yan Wang, Yanqiu Lyu, Jianfeng Mao, Zaiping Guo
The exponential growth of lithium‐ion batteries (LIBs) market driven by electric vehicles has intensified the demand for sustainable and efficient recycling technologies. Among emerging solutions, deep eutectic solvents (DESs) have attracted increasing attention due to their tunable properties, low toxicity, and environmental compatibility. While DESs have been widely applied in the leaching of spent cathodes, their functions and mechanisms remain underexplored. In this review, we critically examine the stage‐specific roles of DESs in the recovery of lithium (Li), nickel (Ni), cobalt (Co), and manganese (Mn) from spent cathodes. DES applications are systematically classified into metal co‐dissolution, single‐metal selectivity (Li‐first, Ni‐first), and two‐metal pairwise separations. We discuss key DES design principles for achieving metal‐specific selectivity, highlighting emerging hydrophobic DESs and redox‐active systems, and expanding roles beyond leaching (binder removal, graphite pre‐concentration, direct regeneration, and hydrophobic DESs for liquid‐liquid extraction). Finally, this review identifies major challenges limiting DES scalability, including viscosity, component stability, recyclability, impurity tolerance, and limited techno‐economic and life cycle analyses. We also propose future directions to fully integrated, closed‐loop, and sustainable DES‐based recycling processes for critical metals. This review provides solvent design and mechanistic insight guidance toward green, selective, and scalable LIB recycling technologies.
{"title":"Stage‐Specific Roles of Deep Eutectic Solvents in Recycling of Spent Lithium‐Ion Batteries","authors":"Jingxiu Wang, Yan Wang, Yanqiu Lyu, Jianfeng Mao, Zaiping Guo","doi":"10.1002/aenm.202506741","DOIUrl":"https://doi.org/10.1002/aenm.202506741","url":null,"abstract":"The exponential growth of lithium‐ion batteries (LIBs) market driven by electric vehicles has intensified the demand for sustainable and efficient recycling technologies. Among emerging solutions, deep eutectic solvents (DESs) have attracted increasing attention due to their tunable properties, low toxicity, and environmental compatibility. While DESs have been widely applied in the leaching of spent cathodes, their functions and mechanisms remain underexplored. In this review, we critically examine the stage‐specific roles of DESs in the recovery of lithium (Li), nickel (Ni), cobalt (Co), and manganese (Mn) from spent cathodes. DES applications are systematically classified into metal co‐dissolution, single‐metal selectivity (Li‐first, Ni‐first), and two‐metal pairwise separations. We discuss key DES design principles for achieving metal‐specific selectivity, highlighting emerging hydrophobic DESs and redox‐active systems, and expanding roles beyond leaching (binder removal, graphite pre‐concentration, direct regeneration, and hydrophobic DESs for liquid‐liquid extraction). Finally, this review identifies major challenges limiting DES scalability, including viscosity, component stability, recyclability, impurity tolerance, and limited techno‐economic and life cycle analyses. We also propose future directions to fully integrated, closed‐loop, and sustainable DES‐based recycling processes for critical metals. This review provides solvent design and mechanistic insight guidance toward green, selective, and scalable LIB recycling technologies.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"30 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146033825","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}
Haodong Wu, Jungjin Yoon, Kavyashree S. Keremane, Luyao Zheng, Yuchen Hou, Shweta Sharma, Dong Yang, Sixing Xiong, Yanhui Zhang, Jin Qian, Shashank Priya, Bed Poudel, Kai Wang
Achieving a simultaneous balance of cost, efficiency, and operational stability is critical for the commercial viability of perovskite photovoltaics. Planar-junction carbon-based perovskite solar modules (C-PSMs) represent a promising platform toward this goal, offering low-cost fabrication and long-term environmental stability enabled by thick carbon electrodes that eliminate the need for encapsulation. However, their power conversion efficiency remains fundamentally limited due to the discontinuous charge percolation and poor heterojunction contact at the carbon/perovskite junction. To overcome these challenges, we present a Holistic Anode Interface Design (H-AID) strategy that integrates two complementary approaches. First, a picosecond laser is used to sculpt a curved perovskite surface morphology, increasing contact area and enhancing charge transfer (Design-1). Second, a gallium-indium eutectic liquid metal is introduced into the carbon paste to fill internal voids and restore conductive pathways (Design-2). Their combination (Design-3) achieves a 42% improvement in module efficiency, reaching 16.88% over a 61.22 cm2 active area, among the highest reported for planar C-PSMs. Moreover, the device retains over 95% of its initial performance after 1200 h under ambient, encapsulated conditions. This work establishes a scalable H-AID framework to unlock cost-efficiency-stability co-optimization in carbon perovskite modules.
{"title":"Holistic Anode Interface Engineering for High-Efficiency and Stable Carbon-Perovskite Solar Modules","authors":"Haodong Wu, Jungjin Yoon, Kavyashree S. Keremane, Luyao Zheng, Yuchen Hou, Shweta Sharma, Dong Yang, Sixing Xiong, Yanhui Zhang, Jin Qian, Shashank Priya, Bed Poudel, Kai Wang","doi":"10.1002/aenm.202506097","DOIUrl":"https://doi.org/10.1002/aenm.202506097","url":null,"abstract":"Achieving a simultaneous balance of cost, efficiency, and operational stability is critical for the commercial viability of perovskite photovoltaics. Planar-junction carbon-based perovskite solar modules (C-PSMs) represent a promising platform toward this goal, offering low-cost fabrication and long-term environmental stability enabled by thick carbon electrodes that eliminate the need for encapsulation. However, their power conversion efficiency remains fundamentally limited due to the discontinuous charge percolation and poor heterojunction contact at the carbon/perovskite junction. To overcome these challenges, we present a Holistic Anode Interface Design (H-AID) strategy that integrates two complementary approaches. First, a picosecond laser is used to sculpt a curved perovskite surface morphology, increasing contact area and enhancing charge transfer (Design-1). Second, a gallium-indium eutectic liquid metal is introduced into the carbon paste to fill internal voids and restore conductive pathways (Design-2). Their combination (Design-3) achieves a 42% improvement in module efficiency, reaching 16.88% over a 61.22 cm<sup>2</sup> active area, among the highest reported for planar C-PSMs. Moreover, the device retains over 95% of its initial performance after 1200 h under ambient, encapsulated conditions. This work establishes a scalable H-AID framework to unlock cost-efficiency-stability co-optimization in carbon perovskite modules.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"49 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022025","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}
Organic redox materials hold great promise for sustainable energy storage due to their structural tunability and elemental abundance. However, their practical application remains hindered by rapid degradation during repeated electrochemical reactions, primarily caused by side processes involving water and unstable redox intermediates. Here, we report a metastable, rehydration-stable molecular capsule formed through the interfacial self-assembly of amphiphilic Pluronic F127 on hydrophobic 2-ethyl-anthraquinone (2-E-AQ) particles. The hydrophobic polypropylene oxide segments anchor onto the 2-E-AQ surface, while the hydrophilic polyethylene oxide chains form a soft, ion-permeable shell that endures drying and reconstructs a gel-like interface upon rehydration, bridging solid-liquid boundaries. Integrated into an aqueous 2-E-AQ||Li2SO4||NaI battery, this soft-interface design stabilizes ion transport and suppresses redox degradation, achieving 99.7% Coulombic efficiency and 85.4% capacity retention after 300 cycles. This work introduces an interface-induced self-assembly paradigm for stabilizing hydrophobic organic redox materials and provides a general framework for constructing adaptive soft interfaces in aqueous electrochemical systems.
{"title":"Self-Assembled Molecular Capsule via Metastable Soft Interface for Stable Aqueous Batteries","authors":"Kaiqiang Zhang, Haoning Xi, Shengtao Yang, Qinhan Yang, Jilei Ye, Yuping Wu","doi":"10.1002/aenm.70668","DOIUrl":"https://doi.org/10.1002/aenm.70668","url":null,"abstract":"Organic redox materials hold great promise for sustainable energy storage due to their structural tunability and elemental abundance. However, their practical application remains hindered by rapid degradation during repeated electrochemical reactions, primarily caused by side processes involving water and unstable redox intermediates. Here, we report a metastable, rehydration-stable molecular capsule formed through the interfacial self-assembly of amphiphilic Pluronic F127 on hydrophobic 2-ethyl-anthraquinone (2-E-AQ) particles. The hydrophobic polypropylene oxide segments anchor onto the 2-E-AQ surface, while the hydrophilic polyethylene oxide chains form a soft, ion-permeable shell that endures drying and reconstructs a gel-like interface upon rehydration, bridging solid-liquid boundaries. Integrated into an aqueous 2-E-AQ||Li<sub>2</sub>SO<sub>4</sub>||NaI battery, this soft-interface design stabilizes ion transport and suppresses redox degradation, achieving 99.7% Coulombic efficiency and 85.4% capacity retention after 300 cycles. This work introduces an interface-induced self-assembly paradigm for stabilizing hydrophobic organic redox materials and provides a general framework for constructing adaptive soft interfaces in aqueous electrochemical systems.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"31 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022028","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}
Clara Schare, Giorgi Titvinidze, Christian Piesold, Edgar Cruz Ortiz, Nodar Dumbadze, Michael Schuster, Klaus‐Dieter Kreuer, Carolin Klose, Andreas Münchinger
Hydrocarbon (HC) membranes have the potential to significantly enhance the efficiency of water electrolyzers. However, their low mechanical integrity under electrolysis conditions, due to severe swelling, poses a challenge for industrial‐scale applications. Here, we present a 12 µm‐thick sulfonated poly(phenylene sulfone) (sPPS) membrane reinforced with a porous polyethylene (PE) substrate. The PE substrate reduces in‐plane swelling by a factor of 7 (10% vs 69%) and improves mechanical stability (440 MPa vs 50 MPa) in water at 60°C. Under electrolysis conditions, a 24 µm thick sandwich of two reinforced membranes shows stable operation over more than 2000 h in a constant current hold at 1 A cm −2 conducted at 60°C (first 1000 h) and 80°C (remaining 1000 h) with only 6 µV h −1 of voltage deviation within the last 500 h. With a potential of 1.67 V and a hydrogen in oxygen content of 1 vol% at 3 A cm −2 , the PFAS‐free membrane clearly outperforms a state‐of‐the‐art reference (Nafion‐N211: 1.73 V and 1.5 vol% at 3 A cm −2 ).
碳氢化合物（HC）膜具有显著提高水电解槽效率的潜力。然而，在电解条件下，由于严重的膨胀，它们的机械完整性很低，这对工业规模的应用提出了挑战。在这里，我们提出了一个12微米厚的磺化聚（苯基砜）（sPPS）膜，用多孔聚乙烯（PE）衬底增强。PE衬底可将平面内膨胀降低7倍（10% vs 69%），并在60°C的水中提高机械稳定性（440 MPa vs 50 MPa）。电解条件下,24µm厚三明治的两个钢筋膜显示稳定运行超过2000 h在恒定电流维持在1厘米−2进行了60°C(前1000 h)和80°C(剩余1000 h)只有6 Vµh−1的电压偏差在过去500 h。1.67 V的潜力和氢气在氧气含量在3厘米−1卷% 2,pfa检测自由膜明显优于高艺术自参考国家优先车道(全氟磺酸N211应承担:1.73 V和1.5 vol % 3厘米−2)。
{"title":"Thin Reinforced Sulfonated Poly(phenylene sulfone) Membranes for Durable Water Electrolysis: Suppressed Swelling and Enhanced Stability Over 2000 Hours","authors":"Clara Schare, Giorgi Titvinidze, Christian Piesold, Edgar Cruz Ortiz, Nodar Dumbadze, Michael Schuster, Klaus‐Dieter Kreuer, Carolin Klose, Andreas Münchinger","doi":"10.1002/aenm.202505888","DOIUrl":"https://doi.org/10.1002/aenm.202505888","url":null,"abstract":"Hydrocarbon (HC) membranes have the potential to significantly enhance the efficiency of water electrolyzers. However, their low mechanical integrity under electrolysis conditions, due to severe swelling, poses a challenge for industrial‐scale applications. Here, we present a 12 µm‐thick sulfonated poly(phenylene sulfone) (sPPS) membrane reinforced with a porous polyethylene (PE) substrate. The PE substrate reduces in‐plane swelling by a factor of 7 (10% vs 69%) and improves mechanical stability (440 MPa vs 50 MPa) in water at 60°C. Under electrolysis conditions, a 24 µm thick sandwich of two reinforced membranes shows stable operation over more than 2000 h in a constant current hold at 1 A cm <jats:sup>−2</jats:sup> conducted at 60°C (first 1000 h) and 80°C (remaining 1000 h) with only 6 µV h <jats:sup>−1</jats:sup> of voltage deviation within the last 500 h. With a potential of 1.67 V and a hydrogen in oxygen content of 1 vol% at 3 A cm <jats:sup>−2</jats:sup> , the PFAS‐free membrane clearly outperforms a state‐of‐the‐art reference (Nafion‐N211: 1.73 V and 1.5 vol% at 3 A cm <jats:sup>−2</jats:sup> ).","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"58 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146014602","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}
Aqueous aluminum-ion batteries are promising for grid-scale energy storage due to their safety, low-cost, and high theoretical specific capacity. However, the development is hindered by the hydrogen evolution reaction from water splitting and corrosion, causing poor reversibility in aluminum plating/stripping. Utilizing strong anti-polyelectrolyte effect from aluminum cations and perchlorate anions, and the outstanding hydration strength from 2-methacryloyloxyethyl phosphorylcholine (MPC), this study introduces a novel polyzwitterionic hydrogel electrolyte (PZHE) for AAIBs with MPC monomer and aluminum perchlorate electrolyte. PZHE binds water molecules under lean-water conditions, greatly reducing free water activity and expanding the electrochemical stability window into 2.5 V. Despite limited water activity, ion migration channels created by zwitterionic phosphorylcholine groups enable high ionic conductivity of 4.22 mS cm−1 at 25°C. Consequently, the PZHE symmetrical cell achieves 600 h of reversible aluminum plating/stripping at a low overpotential of less than 0.2 V. With a potassium nickel hexacyanoferrate (KNHCF) cathode, the coin cell exhibits an initial discharge capacity of 66 mAh g−1 with a 1.2 V voltage plateau and retains 71% capacity after 400 cycles. Additionally, it demonstrates excellent capacity stability in the rest-cycling test (6 months) and pouch cell setup (200 cycles), highlighting its potential for grid-scale energy storage.
水铝离子电池因其安全、低成本和较高的理论比容量而在电网规模的储能中具有广阔的应用前景。但由于水裂解和腐蚀引起的析氢反应阻碍了其发展，导致镀铝/汽提的可逆性较差。利用铝阳离子和高氯酸盐阴离子具有较强的抗聚电解质作用，以及2-甲基丙烯酰氧乙基磷酸胆碱（MPC）具有较强的水合强度，研究了一种以MPC单体和高氯酸铝为电解质的aaib用聚两性离子水凝胶电解质（PZHE）。PZHE在稀水条件下结合水分子，大大降低了自由水活性，并将电化学稳定窗口扩大到2.5 V。尽管水活度有限，但两性磷胆碱基团产生的离子迁移通道在25°C时可实现4.22 mS cm−1的高离子电导率。因此，PZHE对称电池在低于0.2 V的低过电位下实现了600 h的可逆镀铝/剥离。采用六氰镍酸钾（KNHCF）阴极，硬币电池在1.2 V电压平台下的初始放电容量为66 mAh g−1，在400次循环后容量保持71%。此外，它在休息循环测试（6个月）和袋式电池设置（200个循环）中表现出出色的容量稳定性，突出了其在电网规模储能方面的潜力。
{"title":"Mitigating Hydrogen Evolution Reaction with Polyzwitterionic Hydrogel Electrolyte in Aqueous Aluminum-ion Batteries","authors":"Jin-Jie Liew, Bei-Er Jia, Dan-Yang Wang, Ziyue Wen, Hong-Han Choo, Jinxuan Song, Qiang Zhu, Man-Fai Ng, Qingyu Yan","doi":"10.1002/aenm.70677","DOIUrl":"https://doi.org/10.1002/aenm.70677","url":null,"abstract":"Aqueous aluminum-ion batteries are promising for grid-scale energy storage due to their safety, low-cost, and high theoretical specific capacity. However, the development is hindered by the hydrogen evolution reaction from water splitting and corrosion, causing poor reversibility in aluminum plating/stripping. Utilizing strong anti-polyelectrolyte effect from aluminum cations and perchlorate anions, and the outstanding hydration strength from 2-methacryloyloxyethyl phosphorylcholine (MPC), this study introduces a novel polyzwitterionic hydrogel electrolyte (PZHE) for AAIBs with MPC monomer and aluminum perchlorate electrolyte. PZHE binds water molecules under lean-water conditions, greatly reducing free water activity and expanding the electrochemical stability window into 2.5 V. Despite limited water activity, ion migration channels created by zwitterionic phosphorylcholine groups enable high ionic conductivity of 4.22 mS cm<sup>−1</sup> at 25°C. Consequently, the PZHE symmetrical cell achieves 600 h of reversible aluminum plating/stripping at a low overpotential of less than 0.2 V. With a potassium nickel hexacyanoferrate (KNHCF) cathode, the coin cell exhibits an initial discharge capacity of 66 mAh g<sup>−1</sup> with a 1.2 V voltage plateau and retains 71% capacity after 400 cycles. Additionally, it demonstrates excellent capacity stability in the rest-cycling test (6 months) and pouch cell setup (200 cycles), highlighting its potential for grid-scale energy storage.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"66 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146022027","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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