Developing practical zinc (Zn) batteries necessitates taming Zn electrodeposition at source to suppress associated unfavorable reactions while enhancing Zn utilization efficiency at commercially relevant areal capacities (≥10 mAh cm-2). This work overcomes key limitations in Zn utilization (99% in half-cells) and areal capacity through fundamental insights into Zn electrochemistry on tailored current collects. Complementary in-situ characterization and simulations reveal that the tailored brass (Cu0.7Zn0.3) establishes a zincophilic interface, homogeneous electric field distribution, and proton-rejecting properties. This synergy promotes uniform Zn diffusion and progressive nucleation, enabling dendrite-free deposition and effective suppression of water-induced side reactions. The Zn|Brass half-cell achieves an ultrahigh areal capacity of 50 mAh cm-2. In a static Zn-Br2 battery, it delivers 20000 stable cycles at 1 mAh cm-2, while exhibits a scalable areal capacity up to 50 mAh cm-2. A 200 mAh Zn-Br2 pouch cell sustains 1000 cycles, with high reversibility extending to 1000 mAh. The pouch cell offers a practical energy density of 61 Wh kg-1, safe operation, and compatibility with renewable energy integration. This work establishes design guidelines of current collectors for Zn anodes, paving the way for the advancement of practical Zn battery technologies.
开发实用的锌（Zn）电池需要从源头控制锌电沉积，以抑制相关的不良反应，同时提高商业相关面积容量（≥10 mAh cm-2）下锌的利用效率。这项工作克服了锌利用率（半电池中99%）和面积容量的关键限制，通过对锌电化学的基本见解来定制电流收集。互补的原位表征和模拟表明，定制黄铜（Cu0.7Zn0.3）具有亲锌界面、均匀的电场分布和排斥质子的特性。这种协同作用促进锌均匀扩散和渐进成核，使无枝晶沉积和有效抑制水诱导的副反应成为可能。锌|黄铜半电池实现了50毫安时cm-2的超高面积容量。在静态Zn-Br2电池中，它在1 mAh cm-2下提供20000次稳定循环，同时显示可扩展的面积容量高达50 mAh cm-2。一个200毫安时的锌- br2袋电池维持1000次循环，具有高可逆性延伸到1000毫安时。这种袋装电池的实际能量密度为61 Wh kg-1，操作安全，并与可再生能源集成兼容。本工作建立了锌阳极集流器的设计指南，为实用锌电池技术的发展铺平了道路。
{"title":"Taming Zinc Electrodeposition from the Root to Break Zinc Utilization/Capacity Barriers in Practical Zinc Batteries","authors":"Xinhua Zheng, Bibo Han, Chaofan Liu, Ruilin Li, Cheng Chao Li, Shikai Liu, Faxing Wang, Yuping Wu","doi":"10.1039/d5ee05711f","DOIUrl":"https://doi.org/10.1039/d5ee05711f","url":null,"abstract":"Developing practical zinc (Zn) batteries necessitates taming Zn electrodeposition at source to suppress associated unfavorable reactions while enhancing Zn utilization efficiency at commercially relevant areal capacities (≥10 mAh cm-2). This work overcomes key limitations in Zn utilization (99% in half-cells) and areal capacity through fundamental insights into Zn electrochemistry on tailored current collects. Complementary in-situ characterization and simulations reveal that the tailored brass (Cu0.7Zn0.3) establishes a zincophilic interface, homogeneous electric field distribution, and proton-rejecting properties. This synergy promotes uniform Zn diffusion and progressive nucleation, enabling dendrite-free deposition and effective suppression of water-induced side reactions. The Zn|Brass half-cell achieves an ultrahigh areal capacity of 50 mAh cm-2. In a static Zn-Br2 battery, it delivers 20000 stable cycles at 1 mAh cm-2, while exhibits a scalable areal capacity up to 50 mAh cm-2. A 200 mAh Zn-Br2 pouch cell sustains 1000 cycles, with high reversibility extending to 1000 mAh. The pouch cell offers a practical energy density of 61 Wh kg-1, safe operation, and compatibility with renewable energy integration. This work establishes design guidelines of current collectors for Zn anodes, paving the way for the advancement of practical Zn battery technologies.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"8 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145903231","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}
Wejdan Althobaiti, Julien Gorenflot, Catherine S. P. De Castro, Jafar I. Khan, Christopher E. Petoukhoff, Shahidul Alam, Oleksandr Matiash, Yakun He, George T. Harrison, Anirudh Sharma, Weimin Zhang, Valentina Musteata, José P Jurado, Marco Marengo, Derya Baran, Stefaan De Wolf, Iain McCulloch, Shadi Fatayer and Frédéric Laquai
In organic solar cells the energetic landscape of the donor–acceptor heterojunction determines the efficiency of charge generation and charge recombination processes, and thereby the device performance. Here, we present a study on a series of 15 donor–acceptor bulk heterojunctions (BHJs) consisting of either the donor polymer poly(3-hexylthiophene) (P3HT) or poly[2,5-bis(3-tetradecylthiophen-2-yl)thieno[3,2-b]thiophene] (pBTTT-C14) and selected non-fullerene acceptors (NFAs), spanning a wide range of interfacial energetics. We demonstrate that the internal quantum efficiency (IQE) is limited by geminate and non-geminate recombination processes and, importantly, decreases with the energy difference between the donor's ionization energy (IE) and the acceptor's electron affinity (EA), in other words, the diagonal bandgap, specifically if less than 1 eV, regardless of the interfacial IE offset. The dependence of charge recombination on the diagonal bandgap can be explained in the framework of the energy gap law. Our results provide further insight into the importance and impact of interfacial energetics in donor:NFA blends with large IE offsets.
{"title":"Charge recombination in polythiophene: non-fullerene acceptor solar cells with IE offsets exceeding 1 eV","authors":"Wejdan Althobaiti, Julien Gorenflot, Catherine S. P. De Castro, Jafar I. Khan, Christopher E. Petoukhoff, Shahidul Alam, Oleksandr Matiash, Yakun He, George T. Harrison, Anirudh Sharma, Weimin Zhang, Valentina Musteata, José P Jurado, Marco Marengo, Derya Baran, Stefaan De Wolf, Iain McCulloch, Shadi Fatayer and Frédéric Laquai","doi":"10.1039/D5EE05059F","DOIUrl":"10.1039/D5EE05059F","url":null,"abstract":"<p >In organic solar cells the energetic landscape of the donor–acceptor heterojunction determines the efficiency of charge generation and charge recombination processes, and thereby the device performance. Here, we present a study on a series of 15 donor–acceptor bulk heterojunctions (BHJs) consisting of either the donor polymer poly(3-hexylthiophene) (P3HT) or poly[2,5-bis(3-tetradecylthiophen-2-yl)thieno[3,2-<em>b</em>]thiophene] (pBTTT-C14) and selected non-fullerene acceptors (NFAs), spanning a wide range of interfacial energetics. We demonstrate that the internal quantum efficiency (IQE) is limited by geminate and non-geminate recombination processes and, importantly, decreases with the energy difference between the donor's ionization energy (IE) and the acceptor's electron affinity (EA), in other words, the diagonal bandgap, specifically if less than 1 eV, regardless of the interfacial IE offset. The dependence of charge recombination on the diagonal bandgap can be explained in the framework of the energy gap law. Our results provide further insight into the importance and impact of interfacial energetics in donor:NFA blends with large IE offsets.</p>","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":" 2","pages":" 659-679"},"PeriodicalIF":30.8,"publicationDate":"2026-01-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ee/d5ee05059f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145897775","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ultraviolet light-induced degradation (UVID) has been reported across mainstream highefficiency Silicon (Si) solar cell architectures, including heterojunction (HJT), passivated emitter and rear cell (PERC) and tunnel oxide passivated contact (TOPCon) solar cells, causing up to 10% efficiency loss after continuous exposure to high UV doses.Encouragingly, this degradation has also been reported to be recoverable under certain conditions, such as light soaking. However, in the absence of a clear mechanistic understanding of both the degradation and recovery process, current testing protocols and stability metrics fall short of capturing the true UV resilience of these devices. Establishing a fundamental understanding of UVID is therefore critical for developing more predictive testing frameworks and durable cell architectures under real-world operating conditions. In this work, we demonstrate that the UVID of TOPCon silicon solar cells can be effectively recovered using light soaking in the first place. The recoverable macroscopic cell performance is subsequently found correlated with two reversible changes at the materials level: front surface reflectance by optical transmission of SiNx and a Boron-doped Si Raman peak by UV Raman spectroscopy. With further atom probe tomography (APT) investigation and theoretical modeling, the mechanisms of this reversible UVID and light soaking induced recovery (LSIR) process are identified. The elucidation of the reversible UVID mechanism at the atomic level directly informs the development of effective mitigation strategies. We demonstrate that the synchronous use of a thick AlOx film and a low Si:N ratio SiNx layer can improve the UVID resistance of TOPCon solar cells. Moreover, the non-destructive material level characterisation platform established in this work enables effective capture of the degree of UVID resistance in the design of durable TOPCon solar cells with the potential of in-line quality control.
{"title":"A Non-destructive UV Raman Characterisation Platform to Enable Insight into the Mechanism of Reversible Ultraviolet-Induced Degradation (UVID) in TOPCon Solar Cells","authors":"Pengfei Zhang, Caixia Li, Ziheng Liu, Jialiang Huang, Jialin Cong, Jingwen Cao, Kun Yu, Jing Zhou, Liyan Miao, Jingming Zheng, Tingting Li, Jie Yang, Wusong Tao, Xinyu Zhang, Hao Jin, Minglei Sun, Jefferson Zhe Liu, Su-Huai Wei, Martin Green, Xiaojing Hao","doi":"10.1039/d5ee05078b","DOIUrl":"https://doi.org/10.1039/d5ee05078b","url":null,"abstract":"Ultraviolet light-induced degradation (UVID) has been reported across mainstream highefficiency Silicon (Si) solar cell architectures, including heterojunction (HJT), passivated emitter and rear cell (PERC) and tunnel oxide passivated contact (TOPCon) solar cells, causing up to 10% efficiency loss after continuous exposure to high UV doses.Encouragingly, this degradation has also been reported to be recoverable under certain conditions, such as light soaking. However, in the absence of a clear mechanistic understanding of both the degradation and recovery process, current testing protocols and stability metrics fall short of capturing the true UV resilience of these devices. Establishing a fundamental understanding of UVID is therefore critical for developing more predictive testing frameworks and durable cell architectures under real-world operating conditions. In this work, we demonstrate that the UVID of TOPCon silicon solar cells can be effectively recovered using light soaking in the first place. The recoverable macroscopic cell performance is subsequently found correlated with two reversible changes at the materials level: front surface reflectance by optical transmission of SiNx and a Boron-doped Si Raman peak by UV Raman spectroscopy. With further atom probe tomography (APT) investigation and theoretical modeling, the mechanisms of this reversible UVID and light soaking induced recovery (LSIR) process are identified. The elucidation of the reversible UVID mechanism at the atomic level directly informs the development of effective mitigation strategies. We demonstrate that the synchronous use of a thick AlOx film and a low Si:N ratio SiNx layer can improve the UVID resistance of TOPCon solar cells. Moreover, the non-destructive material level characterisation platform established in this work enables effective capture of the degree of UVID resistance in the design of durable TOPCon solar cells with the potential of in-line quality control.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"17 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895458","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}
Ultraviolet light-induced degradation (UVID) has been reported across mainstream highefficiency Silicon (Si) solar cell architectures, including heterojunction (HJT), passivated emitter and rear cell (PERC) and tunnel oxide passivated contact (TOPCon) solar cells, causing up to 10% efficiency loss after continuous exposure to high UV doses.Encouragingly, this degradation has also been reported to be recoverable under certain conditions, such as light soaking. However, in the absence of a clear mechanistic understanding of both the degradation and recovery process, current testing protocols and stability metrics fall short of capturing the true UV resilience of these devices. Establishing a fundamental understanding of UVID is therefore critical for developing more predictive testing frameworks and durable cell architectures under real-world operating conditions. In this work, we demonstrate that the UVID of TOPCon silicon solar cells can be effectively recovered using light soaking in the first place. The recoverable macroscopic cell performance is subsequently found correlated with two reversible changes at the materials level: front surface reflectance by optical transmission of SiNx and a Boron-doped Si Raman peak by UV Raman spectroscopy. With further atom probe tomography (APT) investigation and theoretical modeling, the mechanisms of this reversible UVID and light soaking induced recovery (LSIR) process are identified. The elucidation of the reversible UVID mechanism at the atomic level directly informs the development of effective mitigation strategies. We demonstrate that the synchronous use of a thick AlOx film and a low Si:N ratio SiNx layer can improve the UVID resistance of TOPCon solar cells. Moreover, the non-destructive material level characterisation platform established in this work enables effective capture of the degree of UVID resistance in the design of durable TOPCon solar cells with the potential of in-line quality control.
{"title":"A Non-destructive UV Raman Characterisation Platform to Enable Insight into the Mechanism of Reversible Ultraviolet-Induced Degradation (UVID) in TOPCon Solar Cells","authors":"Pengfei Zhang, Caixia Li, Ziheng Liu, Jialiang Huang, Jialin Cong, Jingwen Cao, Kun Yu, Jing Zhou, Liyan Miao, Jingming Zheng, Tingting Li, Jie Yang, Wusong Tao, Xinyu Zhang, Hao Jin, Minglei Sun, Jefferson Zhe Liu, Su-Huai Wei, Martin Green, Xiaojing Hao","doi":"10.1039/d5ee05078b","DOIUrl":"https://doi.org/10.1039/d5ee05078b","url":null,"abstract":"Ultraviolet light-induced degradation (UVID) has been reported across mainstream highefficiency Silicon (Si) solar cell architectures, including heterojunction (HJT), passivated emitter and rear cell (PERC) and tunnel oxide passivated contact (TOPCon) solar cells, causing up to 10% efficiency loss after continuous exposure to high UV doses.Encouragingly, this degradation has also been reported to be recoverable under certain conditions, such as light soaking. However, in the absence of a clear mechanistic understanding of both the degradation and recovery process, current testing protocols and stability metrics fall short of capturing the true UV resilience of these devices. Establishing a fundamental understanding of UVID is therefore critical for developing more predictive testing frameworks and durable cell architectures under real-world operating conditions. In this work, we demonstrate that the UVID of TOPCon silicon solar cells can be effectively recovered using light soaking in the first place. The recoverable macroscopic cell performance is subsequently found correlated with two reversible changes at the materials level: front surface reflectance by optical transmission of SiNx and a Boron-doped Si Raman peak by UV Raman spectroscopy. With further atom probe tomography (APT) investigation and theoretical modeling, the mechanisms of this reversible UVID and light soaking induced recovery (LSIR) process are identified. The elucidation of the reversible UVID mechanism at the atomic level directly informs the development of effective mitigation strategies. We demonstrate that the synchronous use of a thick AlOx film and a low Si:N ratio SiNx layer can improve the UVID resistance of TOPCon solar cells. Moreover, the non-destructive material level characterisation platform established in this work enables effective capture of the degree of UVID resistance in the design of durable TOPCon solar cells with the potential of in-line quality control.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"122 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2026-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895382","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}
Qin Gao, Can Wang, Nabonswendé Aïda Nadège Ouedraogo, Ke Zhao, Dingqin Hu, Kun Chen, Yi Pan, Zeping Ou, Mingyang Gao, Lei Liu, Junjie Zhang, Teng Gu, Gengsui Tian, Pengyan Zhang, Zeyun Xiao, Haoxuan Guo, Rui Wang, Yujie Zheng, Kuan Sun
Self-assembled monolayers (SAMs) are increasingly utilized as effective hole-collecting material to boost the efficiency of inverted perovskite solar cells (PSCs). However, issues such as incomplete surface coverage and suboptimal interfacial bonding persist, leading to non-radiative recombination and compromise long-term stability. To address these challenges, we developed an innovative strategy by integrating 1-benzyl-3-methylimidazolium tetrafluoroborate (BzMIMBF4) onto the SAM, optimizing the buried interface and enhancing perovskite crystallization. BzMIMBF4 enhances SAM surface coverage through BzMIM+ interactions, forming a robust π-conjugated heterojunction with [4-(3,6-dimethyl-9H-carbazol-9-yl) butyl] phosphonic Acid (Me-4PACz) SAM that optimizes interfacial bonding, inhibits detrimental Pb2+/I- ion migration, and safeguards the bottom electrode. BzMIMBF4 stabilizes crystal nucleation, minimizing defect-related non-radiative recombination, promotes rapid α-phase formation, and enhances (100) plane alignment and charge carrier transfer to the hole-transport layer (HTL). Besides, time-of-flight secondary ion mass spectrometry (ToF-SIMS) depth profiling confirms the distribution of BF4- anions throughout the perovskite film. Simultaneously, BF4- anions effectively passivate perovskite surface and bulk defects, such as uncoordinated Pb2⁺ ions and iodine vacancies, thereby suppressing non-radiative recombination centers. The resulting perovskite films exhibit a pinhole-free structure, increased grain sizes, smoother surfaces, and significantly reduced residual strain. Consequently, BzMIMBF4-treated devices achieve remarkable power conversion efficiencies of up to 26.45% (certified 26.37%) and retain 90.8% of their initial efficiency after 700 hours of operation under one-sun illumination, demonstrating excellent stability. This approach paves the way for high-performance, durable PSCs and their potential in advanced photovoltaic applications.
{"title":"Enhanced interface regulation via π-conjugated heterojunctions for high-efficiency inverted perovskite solar cells","authors":"Qin Gao, Can Wang, Nabonswendé Aïda Nadège Ouedraogo, Ke Zhao, Dingqin Hu, Kun Chen, Yi Pan, Zeping Ou, Mingyang Gao, Lei Liu, Junjie Zhang, Teng Gu, Gengsui Tian, Pengyan Zhang, Zeyun Xiao, Haoxuan Guo, Rui Wang, Yujie Zheng, Kuan Sun","doi":"10.1039/d5ee06342f","DOIUrl":"https://doi.org/10.1039/d5ee06342f","url":null,"abstract":"Self-assembled monolayers (SAMs) are increasingly utilized as effective hole-collecting material to boost the efficiency of inverted perovskite solar cells (PSCs). However, issues such as incomplete surface coverage and suboptimal interfacial bonding persist, leading to non-radiative recombination and compromise long-term stability. To address these challenges, we developed an innovative strategy by integrating 1-benzyl-3-methylimidazolium tetrafluoroborate (BzMIMBF4) onto the SAM, optimizing the buried interface and enhancing perovskite crystallization. BzMIMBF4 enhances SAM surface coverage through BzMIM+ interactions, forming a robust π-conjugated heterojunction with [4-(3,6-dimethyl-9H-carbazol-9-yl) butyl] phosphonic Acid (Me-4PACz) SAM that optimizes interfacial bonding, inhibits detrimental Pb2+/I- ion migration, and safeguards the bottom electrode. BzMIMBF4 stabilizes crystal nucleation, minimizing defect-related non-radiative recombination, promotes rapid α-phase formation, and enhances (100) plane alignment and charge carrier transfer to the hole-transport layer (HTL). Besides, time-of-flight secondary ion mass spectrometry (ToF-SIMS) depth profiling confirms the distribution of BF4- anions throughout the perovskite film. Simultaneously, BF4- anions effectively passivate perovskite surface and bulk defects, such as uncoordinated Pb2⁺ ions and iodine vacancies, thereby suppressing non-radiative recombination centers. The resulting perovskite films exhibit a pinhole-free structure, increased grain sizes, smoother surfaces, and significantly reduced residual strain. Consequently, BzMIMBF4-treated devices achieve remarkable power conversion efficiencies of up to 26.45% (certified 26.37%) and retain 90.8% of their initial efficiency after 700 hours of operation under one-sun illumination, demonstrating excellent stability. This approach paves the way for high-performance, durable PSCs and their potential in advanced photovoltaic applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"90 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-12-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895333","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}
Qiu-Cheng Chen, Wenjin Zhu, Yiqing Chen, Hongmin An, Shuang Yang, Yong Wang, Yali Ji, Guangcan Su, Rui Wang, Jianan Erick Huang, Ji-Yoon Song, Jaerim Kim, Weiyan Ni, Charles Musgrave, Ke Xie, Edward H Sargent
In electrochemical CO reduction reactions, a highly alkaline pH is typically desired to promote multicarbon liquid products and suppress hydrogen evolution, considerations that prioritize pH ≥ 14 (e.g. 1 M KOH). However, bulk electrolytes with pH exceeding 14 are prone to produce corrosion of catalyst and electrolyzer. Here we find that an engineered class of bipolar membrane assemblies (BPMEAs) achieves a superconcentration of local metal hydroxides, and generates a product slate consistent with local electrolyte pH = 15. We report that, in a cathode:anion exchange layer (AEL):cation exchange layer (CEL):anode architecture, a high thickness ratio of CEL:AEL generates a high local pH at the cathode, this achieved by blocking the transport of hydroxide ions, generated on the cathode, over to the anode side. This enables production of C2+ liquids at a total Faradaic efficiency of 93%, with an ethanol:ethylene productivity ratio of 70:1. Compared to anion-exchange membrane assemblies (AEMEAs) operating at the same 100 mA cm-2 current density for similar product selectivity, these BPMEA systems exhibit 28 hours stable operation (compared to <30 minutes in AEMEA), and a 12x lower rate of liquid product crossover, enabling us to report a liquid product concentration of 23 wt% on the cathode. Operando Raman spectroscopy shows that the optimal BPM enhances coverage, on the cathode catalyst, of surface-bound hydroxyl species, ~ 5x higher than AEM systems, simultaneous with maximizing the surface CO population. Mechanistic studies indicate that surface OH promotes hydroxylation of the CCH intermediate, steering the reaction pathway toward ethanol instead of ethylene, leading to the strong preference towards liquid production.
在电化学CO还原反应中，通常需要高碱性pH来促进多碳液体产物和抑制氢的析出，优先考虑pH≥14（例如1 M KOH）。然而，pH值超过14的散装电解质容易对催化剂和电解槽产生腐蚀。在这里，我们发现工程类双极膜组件（bpmea）实现了局部金属氢氧化物的超浓度，并产生了与局部电解质pH = 15一致的产品板岩。我们报道，在阴极：阴离子交换层（AEL）：阳离子交换层（CEL）：阳极结构中，CEL:AEL的高厚度比在阴极产生高局部pH值，这是通过阻止在阴极产生的氢氧根离子向阳极一侧的传输来实现的。这使得C2+液体的总法拉第效率达到93%，乙醇：乙烯的生产比为70:1。与阴离子交换膜组件（AEMEA）相比，在相同的100 mA cm-2电流密度下运行，具有相似的产物选择性，这些BPMEA系统具有28小时的稳定运行（与AEMEA的30分钟相比），并且液体产物交叉率降低了12倍，使我们能够报告阴极上的液体产物浓度为23%。Operando拉曼光谱结果表明，最佳BPM能使阴极催化剂表面结合羟基的覆盖率比AEM体系高5倍，同时使表面CO族数最大化。机理研究表明，表面OH促进CCH中间体的羟基化，使反应途径转向乙醇而不是乙烯，导致强烈的液体生产偏好。
{"title":"High-Asymmetry Bipolar Membrane Electrode Assemblies Generate a Superconcentration of Cations and Hydroxide at a Catalyst Surface","authors":"Qiu-Cheng Chen, Wenjin Zhu, Yiqing Chen, Hongmin An, Shuang Yang, Yong Wang, Yali Ji, Guangcan Su, Rui Wang, Jianan Erick Huang, Ji-Yoon Song, Jaerim Kim, Weiyan Ni, Charles Musgrave, Ke Xie, Edward H Sargent","doi":"10.1039/d5ee04672f","DOIUrl":"https://doi.org/10.1039/d5ee04672f","url":null,"abstract":"In electrochemical CO reduction reactions, a highly alkaline pH is typically desired to promote multicarbon liquid products and suppress hydrogen evolution, considerations that prioritize pH ≥ 14 (e.g. 1 M KOH). However, bulk electrolytes with pH exceeding 14 are prone to produce corrosion of catalyst and electrolyzer. Here we find that an engineered class of bipolar membrane assemblies (BPMEAs) achieves a superconcentration of local metal hydroxides, and generates a product slate consistent with local electrolyte pH = 15. We report that, in a cathode:anion exchange layer (AEL):cation exchange layer (CEL):anode architecture, a high thickness ratio of CEL:AEL generates a high local pH at the cathode, this achieved by blocking the transport of hydroxide ions, generated on the cathode, over to the anode side. This enables production of C2+ liquids at a total Faradaic efficiency of 93%, with an ethanol:ethylene productivity ratio of 70:1. Compared to anion-exchange membrane assemblies (AEMEAs) operating at the same 100 mA cm-2 current density for similar product selectivity, these BPMEA systems exhibit 28 hours stable operation (compared to <30 minutes in AEMEA), and a 12x lower rate of liquid product crossover, enabling us to report a liquid product concentration of 23 wt% on the cathode. Operando Raman spectroscopy shows that the optimal BPM enhances coverage, on the cathode catalyst, of surface-bound hydroxyl species, ~ 5x higher than AEM systems, simultaneous with maximizing the surface CO population. Mechanistic studies indicate that surface OH promotes hydroxylation of the CCH intermediate, steering the reaction pathway toward ethanol instead of ethylene, leading to the strong preference towards liquid production.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"56 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-12-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895332","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}
Anode-free lithium metal batteries hold great promise for high-capacity energy storage by eliminating both the conventional graphite anode and any excess lithium metal. However, irreversible charge-discharge cycles lead to the rapid depletion of active lithium inventories. Moreover, the ether-based electrolytes suited for anode-free configuration are unstable at high voltages, which makes them incompatible with high-nickel cathodes and ultimately curtails their role in enhancing energy density. This study proposes an interface modification strategy driven by helical counter migration. During the formation process, ion movement pathways and anions-cations association effects regulated by internal force generated by a magnetized nickel-coated current collector synergistically guide anions into solvation structures of the adjacent lithium ions migrating in the opposite direction, thereby forming a mechanically robust ion-permeable solid electrolyte interphase, which is characterized by an ordered inorganic particle skeleton infused with organic components, similar to the structure of reinforced concrete. Consequently, the helical counter-directional migration-assisted copper electrode achieves a coulombic efficiency of 99.9%. The assembled anode-free Cu||LiFePO4 cell maintains over 80% capacity retention after 200 cycles, and the anode-less Cu||LiFePO4 cell sustains stable operation for over 1,000 cycles. Furthermore, the internal electric field drives helical counter-directional migration-induced anion-derived solvation sheaths to diffuse to the cathode side and optimize the cathode-electrolyte interphase, enabling stable operation of high-nickel cathodes. The anode-free Cu||NCM811 cells cycled at 4.5 V exhibit a capacity retention exceeding 75% after 100 cycles, and realize a 453.5 Wh kg-1 anode-free lithium metal pouch cell configuration.
{"title":"Helical Counter-Directional Migration-Induced Solvation Sheath Constructing Reinforced Electrode-Electrolyte Interphases for Ultra-Stable Anode-Free Lithium Metal Batteries","authors":"Yunyi Chen, Xitang Qian, Yuxiang Lyu, Yican Qiu, Yee Tung Kwan, Siyu Zhou, Xinyi Lan, Siqi Lu, Minhua Shao","doi":"10.1039/d5ee06208j","DOIUrl":"https://doi.org/10.1039/d5ee06208j","url":null,"abstract":"Anode-free lithium metal batteries hold great promise for high-capacity energy storage by eliminating both the conventional graphite anode and any excess lithium metal. However, irreversible charge-discharge cycles lead to the rapid depletion of active lithium inventories. Moreover, the ether-based electrolytes suited for anode-free configuration are unstable at high voltages, which makes them incompatible with high-nickel cathodes and ultimately curtails their role in enhancing energy density. This study proposes an interface modification strategy driven by helical counter migration. During the formation process, ion movement pathways and anions-cations association effects regulated by internal force generated by a magnetized nickel-coated current collector synergistically guide anions into solvation structures of the adjacent lithium ions migrating in the opposite direction, thereby forming a mechanically robust ion-permeable solid electrolyte interphase, which is characterized by an ordered inorganic particle skeleton infused with organic components, similar to the structure of reinforced concrete. Consequently, the helical counter-directional migration-assisted copper electrode achieves a coulombic efficiency of 99.9%. The assembled anode-free Cu||LiFePO4 cell maintains over 80% capacity retention after 200 cycles, and the anode-less Cu||LiFePO4 cell sustains stable operation for over 1,000 cycles. Furthermore, the internal electric field drives helical counter-directional migration-induced anion-derived solvation sheaths to diffuse to the cathode side and optimize the cathode-electrolyte interphase, enabling stable operation of high-nickel cathodes. The anode-free Cu||NCM811 cells cycled at 4.5 V exhibit a capacity retention exceeding 75% after 100 cycles, and realize a 453.5 Wh kg-1 anode-free lithium metal pouch cell configuration.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"12 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-12-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895203","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 photovoltaics (OPVs) hold unique advantages of light-weight and excellent mechanical flexibility comparing with other PV technologies. Recently, efficiency of OPV has been rapidly progressed to about 20% for small-area rigid devices. Fabricating flexible devices in large area is necessary for OPV technology to move into practical applications with high voltage and power output.High efficiency and high operational stability are required for the upscaled large-area flexible OPV modules. Efficiency and stability are related to device structure, materials (including transparent electrodes, active layers and charge transporting materials), film coating and encapsulation. In this review, we will discuss the progress and basics of large-area high-performance flexible OPV modules, including device structure, efficiency, materials, coating techniques and stability. At the end, we will discuss challenges and outlooks for enhancing the efficiency and stability of the large-area flexible OPV modules.
{"title":"Progress and outlooks of large-area flexible organic photovoltaic modules","authors":"Xinlu Liu, Jiangbin Le, Cong Xie, Xin Lu, Ruiyu Tian, Zedong Xiong, Yinhua Zhou","doi":"10.1039/d5ee06488k","DOIUrl":"https://doi.org/10.1039/d5ee06488k","url":null,"abstract":"Organic photovoltaics (OPVs) hold unique advantages of light-weight and excellent mechanical flexibility comparing with other PV technologies. Recently, efficiency of OPV has been rapidly progressed to about 20% for small-area rigid devices. Fabricating flexible devices in large area is necessary for OPV technology to move into practical applications with high voltage and power output.High efficiency and high operational stability are required for the upscaled large-area flexible OPV modules. Efficiency and stability are related to device structure, materials (including transparent electrodes, active layers and charge transporting materials), film coating and encapsulation. In this review, we will discuss the progress and basics of large-area high-performance flexible OPV modules, including device structure, efficiency, materials, coating techniques and stability. At the end, we will discuss challenges and outlooks for enhancing the efficiency and stability of the large-area flexible OPV modules.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"32 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895205","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}
Liyu Zhu, Hongbin Yang, Kun Liu, Wei Li, Yinjiao Tang, Xiaomin Li, Ting Xu, Lin Dai, Chuanling Si
Growing environmental imperatives are driving the need to substitute petroleum-derived materials with renewable and sustainable alternatives to enable the production of biodegradable and carbon-neutral products. As a naturally abundant and versatile biopolymer, cellulose has been extensively utilized in conventional industries such as papermaking and textiles, and is increasingly being applied in emerging advanced fields, including energy storage, food technology, emulsions, coatings, cosmetics, and biomedical applications. With the iteration and development of energy technology, cellulose-mediated polymer electrolyte materials (PEMs) have re-emerged as the materials of notable scientific and commercial communities due to their exceptional performance advantages in electrochemical energy storage. In this review, we comprehensively summarize and analyze the molecule engineering strategies, key features, and the corresponding construction strategies utilizing cellulose for the preparation of novel PEMs. Particularly, we provide a material and structural perspective how the ion conductivity, ion selectivity, anti-swelling property, self-healing property, flame retardancy, porosity, mechanical property, and photoelectric stability of cellulose-mediated PEMs can be regulated through molecular chemistry. Finally, we examine the potential of these strategies in advancing circular economy principles and environmental sustainability objectives, while also identifying key challenges and outlining promising future research directions. We emphasize the critical need for advanced molecular-level chemical engineering to fully harness the potential of cellulose for energy-related applications.
{"title":"Molecularly Engineered Cellulose: the Next-Generation Sustainable Polymer Electrolyte Materials","authors":"Liyu Zhu, Hongbin Yang, Kun Liu, Wei Li, Yinjiao Tang, Xiaomin Li, Ting Xu, Lin Dai, Chuanling Si","doi":"10.1039/d5ee05398f","DOIUrl":"https://doi.org/10.1039/d5ee05398f","url":null,"abstract":"Growing environmental imperatives are driving the need to substitute petroleum-derived materials with renewable and sustainable alternatives to enable the production of biodegradable and carbon-neutral products. As a naturally abundant and versatile biopolymer, cellulose has been extensively utilized in conventional industries such as papermaking and textiles, and is increasingly being applied in emerging advanced fields, including energy storage, food technology, emulsions, coatings, cosmetics, and biomedical applications. With the iteration and development of energy technology, cellulose-mediated polymer electrolyte materials (PEMs) have re-emerged as the materials of notable scientific and commercial communities due to their exceptional performance advantages in electrochemical energy storage. In this review, we comprehensively summarize and analyze the molecule engineering strategies, key features, and the corresponding construction strategies utilizing cellulose for the preparation of novel PEMs. Particularly, we provide a material and structural perspective how the ion conductivity, ion selectivity, anti-swelling property, self-healing property, flame retardancy, porosity, mechanical property, and photoelectric stability of cellulose-mediated PEMs can be regulated through molecular chemistry. Finally, we examine the potential of these strategies in advancing circular economy principles and environmental sustainability objectives, while also identifying key challenges and outlining promising future research directions. We emphasize the critical need for advanced molecular-level chemical engineering to fully harness the potential of cellulose for energy-related applications.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"36 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145895204","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}
Maoxin Chen, Huan Li, Hui Xu, Zhitan Wu, Jinxing Chen, Huihui Lin, Ao Du, Sundus Umer, Zihui Chen, Ning Yue, Zhijie Yan, Tianyu Yin, Nianjun Yang, Jiong Lu, Weichao Wang, Chunpeng Yang, Quanhong Yang
Zinc–iodine (Zn–I2) batteries are promising for grid-scale energy storage, yet rapid capacity fade from polyiodide shuttling remains a fundamental challenge. This shuttling arises from the coupled, stepwise iodine reduction pathway (*I2 ⇌ *I5 ⇌ *I3 ⇌ *I), wherein conventional single-site catalysts that accelerate the rate-limiting *I3 reduction inevitably stabilize long-chain *I5, exacerbating capacity fading. Herein, we introduce atom-cluster catalysts (ACCs) with tailored atomic geometries that decouple the adsorption energetics of key intermediates. The ACCs destabilize *I5 chain formation while optimizing *I3 reduction kinetics, thereby redirecting the reaction toward a low-barrier *I2 ⇌ *I3 ⇌ *I pathway and suppressing soluble I5− at its source. As a result, Zn1Co ACCs/I2 cathode delivers a high specific capacity of 230.5 mAh g−1 at 6.5 mg cm−2 over 15,000 cycles (2 A g−1). This atomic-scale pathway-engineering strategy resolves the intrinsic trade-off imposed by linear scaling in stepwise conversion reactions and provides a general approach to enabling long-life operation in Zn–I2 batteries and other multi-intermediate electrochemical systems.
锌-碘（Zn-I2）电池有望用于电网规模的储能，但由于多碘化物的穿梭而导致的容量快速衰减仍然是一个根本性的挑战。这种穿梭源于偶联的逐步碘还原途径（*I2 + *I5 + *I3 + *I），其中传统的单位点催化剂加速了限速*I3还原，不可避免地稳定了长链*I5，加剧了容量衰减。在这里，我们引入了原子簇催化剂（ACCs），具有定制的原子几何形状，可以解耦关键中间体的吸附能量。ACCs在优化*I3还原动力学的同时破坏*I5链的形成，从而将反应转向低屏障*I2 + *I3 + *I途径，并从源头抑制可溶性I5−。因此，Zn1Co ACCs/I2阴极在6.5 mg cm−2下提供230.5 mAh g−1的高比容量，超过15,000次循环（2 a g−1）。这种原子尺度的路径工程策略解决了逐步转化反应中线性缩放所带来的内在权衡，并为实现锌- i2电池和其他多中间电化学系统的长寿命运行提供了一种通用方法。
{"title":"Redirecting Iodine Reduction Pathways by Decoupling Adsorption Energies for Long-Life Zn–I2 Batteries","authors":"Maoxin Chen, Huan Li, Hui Xu, Zhitan Wu, Jinxing Chen, Huihui Lin, Ao Du, Sundus Umer, Zihui Chen, Ning Yue, Zhijie Yan, Tianyu Yin, Nianjun Yang, Jiong Lu, Weichao Wang, Chunpeng Yang, Quanhong Yang","doi":"10.1039/d5ee06963g","DOIUrl":"https://doi.org/10.1039/d5ee06963g","url":null,"abstract":"Zinc–iodine (Zn–I<small><sub>2</sub></small>) batteries are promising for grid-scale energy storage, yet rapid capacity fade from polyiodide shuttling remains a fundamental challenge. This shuttling arises from the coupled, stepwise iodine reduction pathway (*I<small><sub>2</sub></small> ⇌ *I<small><sub>5</sub></small> ⇌ *I<small><sub>3</sub></small> ⇌ *I), wherein conventional single-site catalysts that accelerate the rate-limiting *I<small><sub>3</sub></small> reduction inevitably stabilize long-chain *I<small><sub>5</sub></small>, exacerbating capacity fading. Herein, we introduce atom-cluster catalysts (ACCs) with tailored atomic geometries that decouple the adsorption energetics of key intermediates. The ACCs destabilize *I<small><sub>5</sub></small> chain formation while optimizing *I<small><sub>3</sub></small> reduction kinetics, thereby redirecting the reaction toward a low-barrier *I<small><sub>2</sub></small> ⇌ *I<small><sub>3</sub></small> ⇌ *I pathway and suppressing soluble I<small><sub>5</sub></small><small><sup>−</sup></small> at its source. As a result, Zn<small><sub>1</sub></small>Co ACCs/I<small><sub>2</sub></small> cathode delivers a high specific capacity of 230.5 mAh g<small><sup>−1</sup></small> at 6.5 mg cm<small><sup>−2</sup></small> over 15,000 cycles (2 A g<small><sup>−1</sup></small>). This atomic-scale pathway-engineering strategy resolves the intrinsic trade-off imposed by linear scaling in stepwise conversion reactions and provides a general approach to enabling long-life operation in Zn–I<small><sub>2</sub></small> batteries and other multi-intermediate electrochemical systems.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"14 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-12-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145847485","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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