Lithium plating on graphite anodes is a critical degradation pathway in lithium-ion batteries (LIBs), yet quantitative decoupling of its contribution from normal anode aging remains challenging. Here, we designed controlled Li plating tests using negative-to-positive (N/P) ratio < 1 LiFePO4/graphite cells and then compared them with practical fast-charging cells (N/P > 1), quantifying the decomposition of each electrolyte component (solvent, salt, additives) using nuclear magnetic resonance (NMR), mass spectrometry titration (MST), and gas chromatography-mass spectrometry (GC-MS). Controlled Li plating occurs after full graphite lithiation, and it leads to rapid vinylene carbonate (VC) depletion, time-dependent non-Faradaic consumption of hexafluorophosphate (PF6−)/ethyl methyl carbonate (EMC)/ethylene carbonate (EC), and more organic solid-electrolyte interphase (SEI) formation at higher rates. In routine fast-charging aging, Li plating occurs before graphite saturation, and we find pronounced EMC consumption under high-rate conditions compared with low - rate. Our comparative analysis indicates that VC consumption during fast charging originates not only from plating but also significantly from baseline graphite aging. Li plating likely induces SEI rupture, leading to direct contact with electrolyte, thus more organic SEI formation. This quantitative study enables decoupling of Li plating-induced side reactions from general aging without plating, informing battery design and predictive aging models.
{"title":"Decoupling Electrolyte Degradation Pathways With Diverse Li Plating Processes on Graphite Electrodes","authors":"Ke Zhang, Yonggang Hu, Shijun Tang, Wenxuan Hu, Jianrong Lin, Huiyan Zhang, Yufan Peng, Yuanzhe Tao, Yiqing Liao, Ying Lin, Lixuan Pan, Meifang Ding, Jinding Liang, Yimin Wei, Lufeng Yang, Jie Chen, Zhengliang Gong, Yanting Jin, Yong Yang","doi":"10.1002/aenm.202505230","DOIUrl":"https://doi.org/10.1002/aenm.202505230","url":null,"abstract":"Lithium plating on graphite anodes is a critical degradation pathway in lithium-ion batteries (LIBs), yet quantitative decoupling of its contribution from normal anode aging remains challenging. Here, we designed controlled Li plating tests using negative-to-positive (<i>N/P</i>) ratio < 1 LiFePO<sub>4</sub>/graphite cells and then compared them with practical fast-charging cells (<i>N/P</i> > 1), quantifying the decomposition of each electrolyte component (solvent, salt, additives) using nuclear magnetic resonance (NMR), mass spectrometry titration (MST), and gas chromatography-mass spectrometry (GC-MS). Controlled Li plating occurs after full graphite lithiation, and it leads to rapid vinylene carbonate (VC) depletion, time-dependent non-Faradaic consumption of hexafluorophosphate (PF<sub>6</sub><sup>−</sup>)/ethyl methyl carbonate (EMC)/ethylene carbonate (EC), and more organic solid-electrolyte interphase (SEI) formation at higher rates. In routine fast-charging aging, Li plating occurs before graphite saturation, and we find pronounced EMC consumption under high-rate conditions compared with low - rate. Our comparative analysis indicates that VC consumption during fast charging originates not only from plating but also significantly from baseline graphite aging. Li plating likely induces SEI rupture, leading to direct contact with electrolyte, thus more organic SEI formation. This quantitative study enables decoupling of Li plating-induced side reactions from general aging without plating, informing battery design and predictive aging models.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"30 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146005707","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}
Jianchao Gao, Sisi Zhang, Chuang Jiang, Fangming Bai, Jiawei Yan, Wei Liu, Chenxiao Lin, Mingkai Liu
Zinc-ion batteries (ZIBs) have gained considerable attention as sustainable energy storage systems, offering advantages in capacity, safety, and cost. However, issues such as dendrite growth and side reactions hinder their practical adoption. Cellulose-based gel electrolytes (CGEs) have recently emerged as promising materials to mitigate these challenges. By inhibiting zinc dendrite formation and enhancing interfacial stability, CGEs improve cycling longevity and safety in ZIBs. This review begins by classifying gel electrolytes and outlining the distinctive benefits of CGEs prepared via crosslinking and non-crosslinking strategies. It then systematically examines recent developments in CGEs for use with various cathode materials and in multifunctional ZIBs configurations. Finally, the environmental merits and compelling electrochemical properties of CGEs are highlighted, together with a forward-looking discussion on their role in next-generation ZIBs and related future research directions. This work provides a timely and comprehensive resource that integrates materials design with electrochemical insights, offering valuable guidance for the rational development of CGEs.
{"title":"Rational Design of Cellulose-Based Gel Electrolytes for Next-Generation Zinc-Ion Batteries: Mechanisms, Advances, and Perspectives","authors":"Jianchao Gao, Sisi Zhang, Chuang Jiang, Fangming Bai, Jiawei Yan, Wei Liu, Chenxiao Lin, Mingkai Liu","doi":"10.1002/aenm.202506462","DOIUrl":"https://doi.org/10.1002/aenm.202506462","url":null,"abstract":"Zinc-ion batteries (ZIBs) have gained considerable attention as sustainable energy storage systems, offering advantages in capacity, safety, and cost. However, issues such as dendrite growth and side reactions hinder their practical adoption. Cellulose-based gel electrolytes (CGEs) have recently emerged as promising materials to mitigate these challenges. By inhibiting zinc dendrite formation and enhancing interfacial stability, CGEs improve cycling longevity and safety in ZIBs. This review begins by classifying gel electrolytes and outlining the distinctive benefits of CGEs prepared via crosslinking and non-crosslinking strategies. It then systematically examines recent developments in CGEs for use with various cathode materials and in multifunctional ZIBs configurations. Finally, the environmental merits and compelling electrochemical properties of CGEs are highlighted, together with a forward-looking discussion on their role in next-generation ZIBs and related future research directions. This work provides a timely and comprehensive resource that integrates materials design with electrochemical insights, offering valuable guidance for the rational development of CGEs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"47 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001559","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‐ion batteries (LIBs) are the most widely used commercial rechargeable batteries, but the stable supply of key raw materials such as lithium, nickel, and cobalt faces challenges. Sodium‐ion batteries (SIBs) are considered as potential alternatives and complements to LIBs due to similar working principles and the abundance of sodium resources. Layered oxide cathode materials (LOCMs) are recognized as one of the most promising practical cathodes for SIBs because of mature synthesis technology and satisfactory energy density. However, the use of nickel in LOCMs for SIBs has raised concerns about environmental pollution during nickel production and the risk of price volatility stemming from the widespread application of high‐nickel LOCMs for LIBs. Therefore, developing low‐cost nickel‐free LOCMs is crucial for enhancing the environmental friendliness and cost advantages of SIBs. For low‐cost LOCMs, this review discusses the feasibility of replacing Ni 2+ /Ni 4+ with Fe 3+ /Fe 4+ and Mn 3+ /Mn 4+ for charge compensation in SIBs, and summarizes the resulting critical scientific challenges (Fe migration, Mn dissolution, Jahn‐Teller effect, Na deficiency, and thermal instability). Economic efficiency assessment based on cost and electrochemical properties indicates that low‐cost LOCMs exhibit the highest cost‐performance ratio. Finally, to accelerate the commercialization of cost‐effective SIBs technologies, this review outlines promising development pathways of low‐cost LOCMs.
{"title":"Low‐Cost Layered Cathodes Toward Practical Sodium‐Ion Batteries: Scientific Challenges, Resolution Strategies, and Economic Efficiency","authors":"Xu Zhu, Shuai Sun, Mengting Liu, Peng‐Fei Wang","doi":"10.1002/aenm.202506411","DOIUrl":"https://doi.org/10.1002/aenm.202506411","url":null,"abstract":"Lithium‐ion batteries (LIBs) are the most widely used commercial rechargeable batteries, but the stable supply of key raw materials such as lithium, nickel, and cobalt faces challenges. Sodium‐ion batteries (SIBs) are considered as potential alternatives and complements to LIBs due to similar working principles and the abundance of sodium resources. Layered oxide cathode materials (LOCMs) are recognized as one of the most promising practical cathodes for SIBs because of mature synthesis technology and satisfactory energy density. However, the use of nickel in LOCMs for SIBs has raised concerns about environmental pollution during nickel production and the risk of price volatility stemming from the widespread application of high‐nickel LOCMs for LIBs. Therefore, developing low‐cost nickel‐free LOCMs is crucial for enhancing the environmental friendliness and cost advantages of SIBs. For low‐cost LOCMs, this review discusses the feasibility of replacing Ni <jats:sup>2+</jats:sup> /Ni <jats:sup>4+</jats:sup> with Fe <jats:sup>3+</jats:sup> /Fe <jats:sup>4+</jats:sup> and Mn <jats:sup>3+</jats:sup> /Mn <jats:sup>4+</jats:sup> for charge compensation in SIBs, and summarizes the resulting critical scientific challenges (Fe migration, Mn dissolution, Jahn‐Teller effect, Na deficiency, and thermal instability). Economic efficiency assessment based on cost and electrochemical properties indicates that low‐cost LOCMs exhibit the highest cost‐performance ratio. Finally, to accelerate the commercialization of cost‐effective SIBs technologies, this review outlines promising development pathways of low‐cost LOCMs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"183 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001578","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}
Jiwon Kim, Heejun Yun, Yeonseo Kim, Harim Seo, Byeongyun Min, Eunbin Jang, Yeji Yun, Won Jun Choi, Si Hyun Yoon, Heebae Kim, Jeewon Lee, Jeeyoung Yoo, Youn Sang Kim
Among promising lithium salts for electrolyte in lithium‐ion batteries (LIBs), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) forms a more stable inorganic‐rich SEI layer. However, its implementation is limited by severe aluminum current collector corrosion. Since lithium hexafluorophosphate (LiPF 6 ) contributes a stable passivation layer for aluminum, a simply‐mixed LiPF 6 ‐LiTFSI dual‐salt electrolyte offers reduced corrosion. However, its corrosion inhibition capability is not complete. Herein, we propose a SEI‐stabilizing and corrosion‐preventing layer (SCL) that realizes spatial separation of salts, which confines concentrated LiTFSI within a polyethylene glycol dimethacrylate (PEGDMA) network at the anode‐LiPF 6 electrolyte interface. The locally high concentration of LiTFSI in SCL induces a kinetic preference that overrides the thermodynamic preference of LiPF 6 , which enables targeted decomposition of LiTFSI to form a robust SEI layer, while using only a small amount of LiTFSI. Furthermore, SCL demonstrates excellent corrosion‐inhibiting behavior compared to a simply‐mixed LiPF 6 ‐LiTFSI dual‐salt electrolyte. Consequently, SCL enables stable cycling of high‐loading (21.4 mg cm −2 ) practical NCM811/graphite full cells with 93.57% capacity retention after 100 cycles at a high current density of 2.2 mA cm −2 . This strategy enables selective electrochemical reactions through spatial confinement to enhance LIB performance, while suppressing side reactions and reducing costs, providing a scalable approach for next‐generation electrolyte design.
在锂离子电池（lib）电解质中有前途的锂盐中，锂二（三氟甲烷磺酰）亚胺（LiTFSI）形成了更稳定的富含无机元素的SEI层。然而，它的实施受到铝集流器严重腐蚀的限制。由于六氟磷酸锂（lipf6）为铝提供了稳定的钝化层，因此简单混合的lipf6 - LiTFSI双盐电解质可以减少腐蚀。但其缓蚀能力并不完全。在此，我们提出了一种SEI稳定和防腐蚀层（SCL），实现了盐的空间分离，将浓缩的LiTFSI限制在阳极- lipf6电解质界面的聚乙二醇二甲基丙烯酸酯（PEGDMA）网络中。SCL中局部高浓度的LiTFSI诱导了一种动力学偏好，这种偏好超过了lipf6的热力学偏好，这使得LiTFSI能够在仅使用少量LiTFSI的情况下进行有针对性的分解，形成坚固的SEI层。此外，与简单混合的lipf6 - LiTFSI双盐电解质相比，SCL表现出优异的缓蚀性能。因此，SCL能够在2.2 mA cm - 2的高电流密度下稳定循环高负载（21.4 mg cm - 2）实用NCM811/石墨全电池，在100次循环后容量保持率为93.57%。该策略通过空间限制实现选择性电化学反应，以提高LIB性能，同时抑制副反应并降低成本，为下一代电解质设计提供了可扩展的方法。
{"title":"Deriving Stable SEI Layer and Preventing Aluminum Current Collector Corrosion via Preferential Decomposition of Concentrated Lithium Salt for Lithium‐Ion Batteries","authors":"Jiwon Kim, Heejun Yun, Yeonseo Kim, Harim Seo, Byeongyun Min, Eunbin Jang, Yeji Yun, Won Jun Choi, Si Hyun Yoon, Heebae Kim, Jeewon Lee, Jeeyoung Yoo, Youn Sang Kim","doi":"10.1002/aenm.202504436","DOIUrl":"https://doi.org/10.1002/aenm.202504436","url":null,"abstract":"Among promising lithium salts for electrolyte in lithium‐ion batteries (LIBs), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) forms a more stable inorganic‐rich SEI layer. However, its implementation is limited by severe aluminum current collector corrosion. Since lithium hexafluorophosphate (LiPF <jats:sub>6</jats:sub> ) contributes a stable passivation layer for aluminum, a simply‐mixed LiPF <jats:sub>6</jats:sub> ‐LiTFSI dual‐salt electrolyte offers reduced corrosion. However, its corrosion inhibition capability is not complete. Herein, we propose a SEI‐stabilizing and corrosion‐preventing layer (SCL) that realizes spatial separation of salts, which confines concentrated LiTFSI within a polyethylene glycol dimethacrylate (PEGDMA) network at the anode‐LiPF <jats:sub>6</jats:sub> electrolyte interface. The locally high concentration of LiTFSI in SCL induces a kinetic preference that overrides the thermodynamic preference of LiPF <jats:sub>6</jats:sub> , which enables targeted decomposition of LiTFSI to form a robust SEI layer, while using only a small amount of LiTFSI. Furthermore, SCL demonstrates excellent corrosion‐inhibiting behavior compared to a simply‐mixed LiPF <jats:sub>6</jats:sub> ‐LiTFSI dual‐salt electrolyte. Consequently, SCL enables stable cycling of high‐loading (21.4 mg cm <jats:sup>−2</jats:sup> ) practical NCM811/graphite full cells with 93.57% capacity retention after 100 cycles at a high current density of 2.2 mA cm <jats:sup>−2</jats:sup> . This strategy enables selective electrochemical reactions through spatial confinement to enhance LIB performance, while suppressing side reactions and reducing costs, providing a scalable approach for next‐generation electrolyte design.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"10 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001572","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}
Haofu Yuan, Lin Qiao, Shumin Liu, Runhui Li, Yulin Sun, Junchi Zhang, Xiangkun Ma
A bottom‐up relay strategy is first proposed to fabricate integrated dual‐skin‐layer porous membranes (macropore layer between bilateral skin layers) by ingeniously introducing a non‐solvent carrier. Benefiting from the phase inversion relay process, bilateral skin layers can be tailored freely, where ethylene glycol in the non‐solvent carrier effectively regulates the structure of the bottom skin layer by adjusting the ratio of free water to bound water. Thus, a dual‐skin‐layer membrane is designed and applied in a vanadium flow battery (VFB), that features symmetric skin layers (∼600 nm) with sub‐nanometer (∼4.5 Å) pores. The symmetric structure reduces the pressure required for proton migration via the Vehicle mechanism, and the sub‐nanometer pores effectively separate vanadium ions from protons by size exclusion, breaking the trade‐off in traditional membranes. Moreover, the bilateral skin layers protect the macropore layer against the vanadium fouling and mechanical damage. Furthermore, the formation mechanism and ion transport dynamics of the dual‐skin‐layer membrane are analyzed by molecular dynamics and multi‐physical field simulation. As a result, the optimized membrane enables stable VFB operation for over 6000 cycles at 200 mA cm −2 with energy efficiency of ∼83.6%. This work provides an effective approach to prepare integrated symmetric membranes with bilateral skin layers.
首先提出了一种自下而上的接力策略，通过巧妙地引入非溶剂载体来制造集成的双蒙皮层多孔膜（双蒙皮层之间的大孔层）。得益于相变继电器工艺，双侧蒙皮层可以自由定制，其中非溶剂载体中的乙二醇通过调节自由水与结合水的比例有效地调节底层蒙皮层的结构。因此，设计并应用于钒液流电池（VFB）的双蒙皮层膜，具有对称蒙皮层（~ 600 nm）和亚纳米（~ 4.5 Å）孔。对称结构降低了质子通过载体机制迁移所需的压力，亚纳米孔通过尺寸排斥有效地将钒离子从质子中分离出来，打破了传统膜的权衡。此外，双侧皮肤层保护大孔层免受钒污染和机械损伤。通过分子动力学和多物理场模拟分析了双蒙皮膜的形成机理和离子输运动力学。因此，优化后的膜可以在200 mA cm - 2下稳定地运行6000多个循环，能量效率为83.6%。本研究为制备具有双侧皮肤层的一体化对称膜提供了有效的方法。
{"title":"Constructing Integrated Dual‐Skin‐Layer Porous Membranes via a Bottom‐Up Phase Inversion Relay Strategy for Flow Batteries","authors":"Haofu Yuan, Lin Qiao, Shumin Liu, Runhui Li, Yulin Sun, Junchi Zhang, Xiangkun Ma","doi":"10.1002/aenm.202506085","DOIUrl":"https://doi.org/10.1002/aenm.202506085","url":null,"abstract":"A bottom‐up relay strategy is first proposed to fabricate integrated dual‐skin‐layer porous membranes (macropore layer between bilateral skin layers) by ingeniously introducing a non‐solvent carrier. Benefiting from the phase inversion relay process, bilateral skin layers can be tailored freely, where ethylene glycol in the non‐solvent carrier effectively regulates the structure of the bottom skin layer by adjusting the ratio of free water to bound water. Thus, a dual‐skin‐layer membrane is designed and applied in a vanadium flow battery (VFB), that features symmetric skin layers (∼600 nm) with sub‐nanometer (∼4.5 Å) pores. The symmetric structure reduces the pressure required for proton migration via the Vehicle mechanism, and the sub‐nanometer pores effectively separate vanadium ions from protons by size exclusion, breaking the trade‐off in traditional membranes. Moreover, the bilateral skin layers protect the macropore layer against the vanadium fouling and mechanical damage. Furthermore, the formation mechanism and ion transport dynamics of the dual‐skin‐layer membrane are analyzed by molecular dynamics and multi‐physical field simulation. As a result, the optimized membrane enables stable VFB operation for over 6000 cycles at 200 mA cm <jats:sup>−</jats:sup> <jats:sup>2</jats:sup> with energy efficiency of ∼83.6%. This work provides an effective approach to prepare integrated symmetric membranes with bilateral skin layers.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"10 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001579","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}
Globally, the proton exchange membrane water electrolyzers (PEMWEs) already account for approximately 30% of the hydrogen market and are undergoing rapid expansion. However, the commercially used iridium-based anodic oxygen evolution reaction (OER) catalysts in PEMWEs still suffer from notably poor reactivity. At present, the oxide pathway mechanism (OPM) is an important route to achieve both high activity and durability in OER. Nevertheless, the performance of conventional Ir-based crystalline OER catalysts following the OPM pathway remains far below their theoretical limit, which is significantly hindered by two intrinsic limitations. First, their rigid lattice structures prevent the shortening of metal-metal distances, which is essential to facilitate the rate-determining O*─O* dimerization. Second, the repulsion between O* adsorbates during OER inevitably weakens the metal = O* bond and undermines the overall oxygen evolution efficiency. Herein, we report that an amorphous IrMOx catalyst elegantly overcomes the limitations of the OPM pathway by virtue of its dynamic surface structure and strong oxophilicity of M. The dynamic surface structure promotes O*─O* coupling, while the oxophilic nature of M compensates for the inherent weakening of the metal = O* bond during OER. Because of that, the catalyst exhibits outstanding OER performance, along with excellent catalytic durability over 1200 h’ PEM testing.
在全球范围内，质子交换膜水电解槽（PEMWEs）已经占据了大约30%的氢气市场，并且正在快速扩张。然而，工业上使用的铱基阳极析氧反应（OER）催化剂的反应活性仍然很差。目前，氧化途径机制（OPM）是实现OER高活性和耐久性的重要途径。然而，遵循OPM途径的传统ir基晶体OER催化剂的性能仍然远远低于其理论极限，这受到两个内在限制的显著阻碍。首先，它们的刚性晶格结构阻止了金属-金属距离的缩短，这对于促进决定速率的O*─O*二聚化至关重要。其次，OER过程中O*吸附之间的斥力不可避免地削弱了金属= O*键，破坏了整体的析氧效率。本文中，我们报道了一种无定形IrMOx催化剂凭借其动态表面结构和M的强亲氧性，巧妙地克服了OPM途径的局限性。动态表面结构促进了O*─O*耦合，而M的亲氧性补偿了OER过程中金属= O*键的固有弱化。因此，该催化剂表现出出色的OER性能，以及超过1200 h PEM测试的优异催化耐久性。
{"title":"Structure Disorder-Induced Dynamic Oxophilic Surface Boosting O* Radical Dimerization for Superior Acid Oxygen Evolution","authors":"Xianghui Shi, Zhihao Zhang, Liuxin Xu, Zhe Wang, Qianjiang Mao, Yue Jiang, Xiaoxin Yang, Zihao Ma, Dan Cheng, Wenkun Jiang, Mingzhen Hu, Kebin Zhou","doi":"10.1002/aenm.202506570","DOIUrl":"https://doi.org/10.1002/aenm.202506570","url":null,"abstract":"Globally, the proton exchange membrane water electrolyzers (PEMWEs) already account for approximately 30% of the hydrogen market and are undergoing rapid expansion. However, the commercially used iridium-based anodic oxygen evolution reaction (OER) catalysts in PEMWEs still suffer from notably poor reactivity. At present, the oxide pathway mechanism (OPM) is an important route to achieve both high activity and durability in OER. Nevertheless, the performance of conventional Ir-based crystalline OER catalysts following the OPM pathway remains far below their theoretical limit, which is significantly hindered by two intrinsic limitations. First, their rigid lattice structures prevent the shortening of metal-metal distances, which is essential to facilitate the rate-determining O<sup>*</sup>─O<sup>*</sup> dimerization. Second, the repulsion between O<sup>*</sup> adsorbates during OER inevitably weakens the metal = O<sup>*</sup> bond and undermines the overall oxygen evolution efficiency. Herein, we report that an amorphous IrMO<sub>x</sub> catalyst elegantly overcomes the limitations of the OPM pathway by virtue of its dynamic surface structure and strong oxophilicity of M. The dynamic surface structure promotes O<sup>*</sup>─O<sup>*</sup> coupling, while the oxophilic nature of M compensates for the inherent weakening of the metal = O<sup>*</sup> bond during OER. Because of that, the catalyst exhibits outstanding OER performance, along with excellent catalytic durability over 1200 h’ PEM testing.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"5 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001564","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}
Sangyeop Lee, Suyun Chae, Hyeongseok Shim, Yubin Lee, Dong‐Yeob Han, Sinho Choi, Gyujin Song, Donghwa Lee, Soojin Park
Sustainable electrification continues to drive growing interest in high‐performance lithium‐ion batteries (LIBs), which are essential energy storage systems for this transition. However, conventional graphite‐based LIBs cannot meet the stringent requirements of next‐generation applications, necessitating advanced alternatives. Herein, we report the design of fluorine‐incorporated silicon (FIS) nanostructures through a novel solid–vapor–solid synthesis method that integrates metallothermic reduction with combined top‐down and bottom‐up processes. Crucially, fluorine (F) atoms are inherently positioned both at interstitial sites within the silicon (Si) lattice and on the particle surface. Interstitial F modifies the direct‐allowed band structure of Si and expands lithium penetration pathways, thereby enhancing charge transport through improved electronic conductivity and ion migration. Meanwhile, surface‐bound F induces superhydrophobicity, enabling hydrofluoric acid‐free processing during both synthesis and electrode fabrication. Comprehensively, unveiled features of FIS offer a cost‐effective manufacturing, improved structural and electrochemical stability, and superior performance, leading to cycle‐stable, fast‐charging Si anodes for advanced LIBs.
{"title":"Geometric Remodeling of Silicon Crystal Structure Through Atomic‐Level Fluorine Incorporation for High‐Performance Lithium‐Ion Batteries","authors":"Sangyeop Lee, Suyun Chae, Hyeongseok Shim, Yubin Lee, Dong‐Yeob Han, Sinho Choi, Gyujin Song, Donghwa Lee, Soojin Park","doi":"10.1002/aenm.202504961","DOIUrl":"https://doi.org/10.1002/aenm.202504961","url":null,"abstract":"Sustainable electrification continues to drive growing interest in high‐performance lithium‐ion batteries (LIBs), which are essential energy storage systems for this transition. However, conventional graphite‐based LIBs cannot meet the stringent requirements of next‐generation applications, necessitating advanced alternatives. Herein, we report the design of fluorine‐incorporated silicon (FIS) nanostructures through a novel solid–vapor–solid synthesis method that integrates metallothermic reduction with combined top‐down and bottom‐up processes. Crucially, fluorine (F) atoms are inherently positioned both at interstitial sites within the silicon (Si) lattice and on the particle surface. Interstitial F modifies the direct‐allowed band structure of Si and expands lithium penetration pathways, thereby enhancing charge transport through improved electronic conductivity and ion migration. Meanwhile, surface‐bound F induces superhydrophobicity, enabling hydrofluoric acid‐free processing during both synthesis and electrode fabrication. Comprehensively, unveiled features of FIS offer a cost‐effective manufacturing, improved structural and electrochemical stability, and superior performance, leading to cycle‐stable, fast‐charging Si anodes for advanced LIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"108 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001573","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}
MXene‐based proton pseudocapacitors are promising candidates for microscale electronic devices due to their superior portability and high‐power density, yet their advancement is constrained by the scarcity of efficient electrode materials. Herein, a nitrogen‐directed Ti 3 C 2 T x MXene with substitution of terminal functional groups by nitrogen is proposed as a high‐efficiency electrode material for proton pseudocapacitors. This strategy introduces multiple surface‐active sites and a new pathway for fast proton storage for achieving high specific capacitance. Impressively, a nitrogen‐directed proton storage mechanism is unraveled in the terminal N groups can preferentially interact with protons and lower the diffusion energy barrier toward adjacent active‐sites, substantially facilitating the storage of protons. As a result, the N300‐Ti 3 C 2 T x delivers excellent capacitance retention of 84.48% after 30,000 cycles at 2 A g −1 . Furthermore, in‐plane proton pseudocapacitors are fabricated via direct ink writing, which shows great compatibility with various connection configurations, validating the superior potential in application feasibility of the N‐directed Ti 3 C 2 T x on proton storage.
基于MXene的质子假电容器由于其优越的便携性和高功率密度而成为微尺度电子器件的有希望的候选者，但其发展受到高效电极材料的缺乏的限制。本文提出了一种末端官能团被氮取代的氮定向Ti 3c2txmxene作为质子假电容器的高效电极材料。该策略引入了多个表面活性位点和快速质子存储的新途径，以实现高比电容。令人印象深刻的是，在末端N基团中揭示了氮定向质子存储机制，可以优先与质子相互作用，并降低向邻近活性位点的扩散能垒，从而大大促进了质子的存储。因此，在2 a g−1下，N300‐ti3c2tx在30,000次循环后提供了84.48%的优异电容保持率。此外，通过直接墨水写入制备了平面内质子假电容器，该电容器与各种连接结构具有良好的兼容性，验证了N -取向Ti - 3c2tx在质子存储方面的应用可行性。
{"title":"Nitrogen‐Directed Ti 3 C 2 T x Enabling Rapid Proton Storage for Printed in‐Plane Micro‐Pseudocapacitors","authors":"Duo Chen, Xu Jiang, Xinji Zhou, Chenglin Miao, Tengyu Yao, Wentong Shen, Tiezhu Xu, Honghui Gu, Laifa Shen","doi":"10.1002/aenm.202505587","DOIUrl":"https://doi.org/10.1002/aenm.202505587","url":null,"abstract":"MXene‐based proton pseudocapacitors are promising candidates for microscale electronic devices due to their superior portability and high‐power density, yet their advancement is constrained by the scarcity of efficient electrode materials. Herein, a nitrogen‐directed Ti <jats:sub>3</jats:sub> C <jats:sub>2</jats:sub> T <jats:sub>x</jats:sub> MXene with substitution of terminal functional groups by nitrogen is proposed as a high‐efficiency electrode material for proton pseudocapacitors. This strategy introduces multiple surface‐active sites and a new pathway for fast proton storage for achieving high specific capacitance. Impressively, a nitrogen‐directed proton storage mechanism is unraveled in the terminal N groups can preferentially interact with protons and lower the diffusion energy barrier toward adjacent active‐sites, substantially facilitating the storage of protons. As a result, the N300‐Ti <jats:sub>3</jats:sub> C <jats:sub>2</jats:sub> T <jats:sub>x</jats:sub> delivers excellent capacitance retention of 84.48% after 30,000 cycles at 2 A g <jats:sup>−1</jats:sup> . Furthermore, in‐plane proton pseudocapacitors are fabricated via direct ink writing, which shows great compatibility with various connection configurations, validating the superior potential in application feasibility of the N‐directed Ti <jats:sub>3</jats:sub> C <jats:sub>2</jats:sub> T <jats:sub>x</jats:sub> on proton storage.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"44 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001575","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}
Mengli Liu, Yongqi Bai, Ran Su, Jingyu Shi, Ze Jin, Chen Shen, Haotian Hu, Quan Liu, Ziyi Ge
Overcoming the inherent trade‐off between near‐infrared photon harvesting and high open‐circuit voltage losses in bulk‐heterojunction blends is critical for advancing semi‐transparent organic solar cells (ST‐OSC). Herein, we present a molecular design that combines vinylene π ‐bridge incorporation and terminal‐group halogenation to tailor energy level alignment and blend morphology with PCE10 donor. These designed materials (eC9‐V‐2Cl(‐4Cl) and eC9‐DV‐2Cl) exhibit broadened NIR absorption (up to 1020 nm) and significantly reduce non‐radiative recombination voltage loss by a maximum of ∼100 mV compared to the standard PCE10:BTP‐eC9 device. The optimized PCE10:eC9‐V‐2Cl blend, processed from a green solvent in an inverted structure, achieves a remarkable power conversion efficiency (PCE) of 14.2% for opaque devices with a minimal voltage loss of ∼250 mV. Furthermore, a simply 1D double‐layered nano‐photoinc structure (LiF/MoO 3 ) as an optical out‐coupling layer was integrated into the ST‐OSC, delivering a PCE of 9.9% with an average visible transmittance (AVT) of 42.6%, and yielding a light utilization efficiency (LUE) of 4.3%. Scaling to 5 × 5 cm 2 ST‐OSC modules, an active‐area efficiency of ≈9% was reached with a remarkably high geometric fill factor of 96.5%. These findings provide new molecular design principles for high‐performance ST‐OSCs, making these devices highly attractive for sustainable and scalable applications like energy‐saving agrivoltaic systems and aesthetically transparent solar windows.
{"title":"Molecular Engineering of Asymmetric Narrow‐Gap Acceptors for High‐Performance Semitransparent Organic Solar Cells and Modules with Minimized Energy Losses","authors":"Mengli Liu, Yongqi Bai, Ran Su, Jingyu Shi, Ze Jin, Chen Shen, Haotian Hu, Quan Liu, Ziyi Ge","doi":"10.1002/aenm.202505706","DOIUrl":"https://doi.org/10.1002/aenm.202505706","url":null,"abstract":"Overcoming the inherent trade‐off between near‐infrared photon harvesting and high open‐circuit voltage losses in bulk‐heterojunction blends is critical for advancing semi‐transparent organic solar cells (ST‐OSC). Herein, we present a molecular design that combines vinylene <jats:italic>π</jats:italic> ‐bridge incorporation and terminal‐group halogenation to tailor energy level alignment and blend morphology with PCE10 donor. These designed materials (eC9‐V‐2Cl(‐4Cl) and eC9‐DV‐2Cl) exhibit broadened NIR absorption (up to 1020 nm) and significantly reduce non‐radiative recombination voltage loss by a maximum of ∼100 mV compared to the standard PCE10:BTP‐eC9 device. The optimized PCE10:eC9‐V‐2Cl blend, processed from a green solvent in an inverted structure, achieves a remarkable power conversion efficiency (PCE) of 14.2% for opaque devices with a minimal voltage loss of ∼250 mV. Furthermore, a simply 1D double‐layered nano‐photoinc structure (LiF/MoO <jats:sub>3</jats:sub> ) as an optical out‐coupling layer was integrated into the ST‐OSC, delivering a PCE of 9.9% with an average visible transmittance (AVT) of 42.6%, and yielding a light utilization efficiency (LUE) of 4.3%. Scaling to 5 × 5 cm <jats:sup>2</jats:sup> ST‐OSC modules, an active‐area efficiency of ≈9% was reached with a remarkably high geometric fill factor of 96.5%. These findings provide new molecular design principles for high‐performance ST‐OSCs, making these devices highly attractive for sustainable and scalable applications like energy‐saving agrivoltaic systems and aesthetically transparent solar windows.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"47 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001574","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}
Yuxin Tang, Nan-Nan Liang, Yinghui Li, Qingliang Luo, Wei Ding, Biao Li, Xin Gao, Quanquan Pang, Dongxiao Ji, Mingchuan Luo
While Kirkendall oxidation (KO) facilely fabricates transition metal oxides for oxygen evolution reaction (OER) in proton exchange membrane water electrolyzers (PEMWEs), it concomitantly triggers detrimental lattice expansion. For Co3O4, an appealing IrO2-alternative catalyst, KO generates a free lattice expansion above 2.4%, resulting in suboptimal activity and stability. Here, we design a confined KO approach and coat the precursor Co nanoparticles with atomic carbon layers, enabling controllable lattice expansion of Co3O4 between 0.2% and 1.8%. For the first time, a strain-dependent OER activity of Co3O4 is established in acidic media, with an expansion strain of 1.4% exhibiting the lowest overpotential of 377 mV at 10 mA cm−2. Synchrotron X-ray absorption spectroscopies and theoretical calculations unravel the adjustable lattice strain regulates the d-band center of Co sites and further modifies the oxygenate adsorptions. When integrated into a PEMWE, the 1.4%-strained Co3O4 catalyst sustainably operates at 250 mA cm−2 over 100 h. The reported confined KO provides a new means for strain engineering of transition metal oxides for energy electrocatalysis.
虽然Kirkendall氧化（KO）很容易在质子交换膜水电解槽（PEMWEs）中制造出析氧反应（OER）的过渡金属氧化物，但它同时引发了有害的晶格膨胀。Co3O4是一种很有吸引力的iro2替代催化剂，KO产生的自由晶格膨胀率在2.4%以上，导致活性和稳定性不理想。在这里，我们设计了一种受限的KO方法，并在前驱体Co纳米颗粒上包裹了原子碳层，使Co3O4的晶格膨胀在0.2%到1.8%之间可控。首次在酸性介质中建立了菌株依赖的Co3O4 OER活性，膨胀菌株为1.4%，在10 mA cm−2下过电位最低，为377 mV。同步加速器x射线吸收光谱和理论计算揭示了可调晶格应变调节Co位的d波段中心，并进一步改变了氧合物的吸附。当集成到PEMWE中时，1.4%应变的Co3O4催化剂在250 mA cm−2下持续工作100小时。报道的受限KO为能源电催化过渡金属氧化物的应变工程提供了一种新的手段。
{"title":"Confined Kirkendall Strain Engineering Promotes Oxygen Evolution on Co3O4 for Proton Exchange Membrane Water Electrolyzer","authors":"Yuxin Tang, Nan-Nan Liang, Yinghui Li, Qingliang Luo, Wei Ding, Biao Li, Xin Gao, Quanquan Pang, Dongxiao Ji, Mingchuan Luo","doi":"10.1002/aenm.202506692","DOIUrl":"https://doi.org/10.1002/aenm.202506692","url":null,"abstract":"While Kirkendall oxidation (KO) facilely fabricates transition metal oxides for oxygen evolution reaction (OER) in proton exchange membrane water electrolyzers (PEMWEs), it concomitantly triggers detrimental lattice expansion. For Co<sub>3</sub>O<sub>4</sub>, an appealing IrO<sub>2</sub>-alternative catalyst, KO generates a free lattice expansion above 2.4%, resulting in suboptimal activity and stability. Here, we design a confined KO approach and coat the precursor Co nanoparticles with atomic carbon layers, enabling controllable lattice expansion of Co<sub>3</sub>O<sub>4</sub> between 0.2% and 1.8%. For the first time, a strain-dependent OER activity of Co<sub>3</sub>O<sub>4</sub> is established in acidic media, with an expansion strain of 1.4% exhibiting the lowest overpotential of 377 mV at 10 mA cm<sup>−2</sup>. Synchrotron X-ray absorption spectroscopies and theoretical calculations unravel the adjustable lattice strain regulates the d-band center of Co sites and further modifies the oxygenate adsorptions. When integrated into a PEMWE, the 1.4%-strained Co<sub>3</sub>O<sub>4</sub> catalyst sustainably operates at 250 mA cm<sup>−2</sup> over 100 h. The reported confined KO provides a new means for strain engineering of transition metal oxides for energy electrocatalysis.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"266 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001563","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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