Large-area perovskite light-emitting diodes (LEDs) remain limited by severe performance losses arising from grain boundary defects and nonuniform film formation. Here we introduce a ZnBr2-mediated crystallization strategy that selectively passivates grain boundary defects while inducing the in situ formation of the wide-bandgap Cs2ZnBr4 interphase. This intergranular phase bridges adjacent CsPbBr3 grains, suppressing trap-assisted recombination, directing preferential crystal orientation, and enhancing environmental stability. Leveraging this approach, we realize large-area quasi-2D perovskite LEDs (active area: 225 mm2) exhibiting record-high external quantum efficiencies (EQEs) of 25.2% for green emission at 516 nm and 23.7% for red emission at 640 nm, which are the highest reported to date for devices of this scale. These results establish intergranular phase engineering as an effective and generalizable route to overcome intrinsic scaling challenges in quasi-2D perovskites, paving the way for efficient, stable, and manufacturable perovskite light-emitting technologies.
{"title":"Bridging Grains with Cs2ZnBr4 Enables Record 25.2% EQE Large-Area Perovskite LEDs","authors":"Yulu Hua, Zhenduo Wang, Shichao Zhen, Wei Dong, Yingtong Zhou, Shuo Li, Ziqi Song, Zeyu Miao, Zhijian Li, Xihe Xu, Changlei Wang, Yunan Gao, Wenxu Yin, Bo Gao, Di Li, Xiaoyu Zhang, Weitao Zheng","doi":"10.1021/acsenergylett.6c00048","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c00048","url":null,"abstract":"Large-area perovskite light-emitting diodes (LEDs) remain limited by severe performance losses arising from grain boundary defects and nonuniform film formation. Here we introduce a ZnBr<sub>2</sub>-mediated crystallization strategy that selectively passivates grain boundary defects while inducing the in situ formation of the wide-bandgap Cs<sub>2</sub>ZnBr<sub>4</sub> interphase. This intergranular phase bridges adjacent CsPbBr<sub>3</sub> grains, suppressing trap-assisted recombination, directing preferential crystal orientation, and enhancing environmental stability. Leveraging this approach, we realize large-area quasi-2D perovskite LEDs (active area: 225 mm<sup>2</sup>) exhibiting record-high external quantum efficiencies (EQEs) of 25.2% for green emission at 516 nm and 23.7% for red emission at 640 nm, which are the highest reported to date for devices of this scale. These results establish intergranular phase engineering as an effective and generalizable route to overcome intrinsic scaling challenges in quasi-2D perovskites, paving the way for efficient, stable, and manufacturable perovskite light-emitting technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"74 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072522","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}
Pub Date : 2026-01-29DOI: 10.1021/acsenergylett.5c03780
Karen van den Akker, Hassan Javed, Julia Fernández-Vidal, Onno van der Heijden, Kees E. Kolmeijer, Rik V. Mom, Marc T. M. Koper
The kinetics of alkaline water reduction on Pt can be strongly affected by the accumulation of impurities on the surface. Here, we demonstrate that such impurity effects can play a role even when the highest purity, pretreated NaOH electrolyte is used, which can lead to a misinterpretation of hydrogen evolution reaction (HER) activity trends. We show that the impurity accumulation time of a chosen electrochemical protocol plays a crucial role in the extent of surface contamination and the resulting drift in HER current. By incorporating intermittent surface cleaning into the measurement sequence, we effectively mitigated contamination accumulation effects. However, the HER activity still largely depends on the electrolyte impurity levels. We argue, therefore, that optimization of both the measurement method and the purity of the chemicals is essential for minimizing contamination effects and provide recommendations for employing this integrated approach to prevent systematic errors.
{"title":"Minimizing the Influence of Metal Contaminations for the Alkaline Hydrogen Evolution Reaction on Platinum","authors":"Karen van den Akker, Hassan Javed, Julia Fernández-Vidal, Onno van der Heijden, Kees E. Kolmeijer, Rik V. Mom, Marc T. M. Koper","doi":"10.1021/acsenergylett.5c03780","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03780","url":null,"abstract":"The kinetics of alkaline water reduction on Pt can be strongly affected by the accumulation of impurities on the surface. Here, we demonstrate that such impurity effects can play a role even when the highest purity, pretreated NaOH electrolyte is used, which can lead to a misinterpretation of hydrogen evolution reaction (HER) activity trends. We show that the impurity accumulation time of a chosen electrochemical protocol plays a crucial role in the extent of surface contamination and the resulting drift in HER current. By incorporating intermittent surface cleaning into the measurement sequence, we effectively mitigated contamination accumulation effects. However, the HER activity still largely depends on the electrolyte impurity levels. We argue, therefore, that optimization of both the measurement method and the purity of the chemicals is essential for minimizing contamination effects and provide recommendations for employing this integrated approach to prevent systematic errors.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"1 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097857","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}
Pub Date : 2026-01-29DOI: 10.1021/acsenergylett.6c00026
Dong-Min Kim, Gan Chen, Michael A. Baird, Livia Pugens Matte, Youngmin Ko, Carson O. Zellmann-Parrotta, Jiwoong Bae, Zhaoyang Chen, Yan Yao, Mary C. Scott, Ying Chen, Brett A. Helms
Solid-state sodium metal batteries (SSBs) are candidates for TWh-scale energy storage systems, yet remain challenged by poor processability, cracking, and interface incoherence between inorganic electrolytes and cathodes. Here, we architect thermoformable organo–ionic (ORION) electrolytes comprising controllably clustered ion aggregates within a zwitterionic matrix to create SSBs with organic cathodes. ORION electrolytes are viscoelastic liquids above 110 °C, yet they are viscoelastic solids at typical battery operating temperatures, which overcome the aforementioned challenges. We introduced ether ligands to tailor Na+-ion coordination environments and transport over 3 orders of magnitude (3.4 × 10–3 – 1.0 mS cm–1), whereupon we observed monotonic increases in Na+ mobility with increasing coordination number (up to 2.5); yet the fraction of mobile ions decreased. Thus, ligands dissociate Na+ from larger ion clusters and aggregates, prescribe what the effective mass of Na+ will be, and how Na+ will move within the zwitterionic matrix via vehicular diffusion.
固态钠金属电池（SSBs）是太瓦时规模储能系统的候选材料，但仍面临着加工性能差、开裂以及无机电解质与阴极之间界面不连贯等问题的挑战。在这里，我们设计了热成型有机离子（ORION）电解质，包括在两性离子基质中可控制聚集的离子聚集体，以创建具有有机阴极的ssb。ORION电解质在110°C以上为粘弹性液体，但在典型电池工作温度下，它们是粘弹性固体，克服了上述挑战。我们引入了醚配体来调整Na+离子配位环境，并在3个数量级（3.4 × 10-3 - 1.0 mS cm-1）内传输，因此我们观察到Na+迁移率随着配位数的增加而单调增加（高达2.5）；然而，可移动离子的比例减少了。因此，配体将Na+从较大的离子团簇和聚集体中解离，规定Na+的有效质量是多少，以及Na+如何通过载体扩散在两性离子基质中移动。
{"title":"Thermoformable Electrolytes for Solid-State Sodium Metal Batteries Employing Organic Cathodes","authors":"Dong-Min Kim, Gan Chen, Michael A. Baird, Livia Pugens Matte, Youngmin Ko, Carson O. Zellmann-Parrotta, Jiwoong Bae, Zhaoyang Chen, Yan Yao, Mary C. Scott, Ying Chen, Brett A. Helms","doi":"10.1021/acsenergylett.6c00026","DOIUrl":"https://doi.org/10.1021/acsenergylett.6c00026","url":null,"abstract":"Solid-state sodium metal batteries (SSBs) are candidates for TWh-scale energy storage systems, yet remain challenged by poor processability, cracking, and interface incoherence between inorganic electrolytes and cathodes. Here, we architect thermoformable organo–ionic (ORION) electrolytes comprising controllably clustered ion aggregates within a zwitterionic matrix to create SSBs with organic cathodes. ORION electrolytes are viscoelastic liquids above 110 °C, yet they are viscoelastic solids at typical battery operating temperatures, which overcome the aforementioned challenges. We introduced ether ligands to tailor Na<sup>+</sup>-ion coordination environments and transport over 3 orders of magnitude (3.4 × 10<sup>–3</sup> – 1.0 mS cm<sup>–1</sup>), whereupon we observed monotonic increases in Na<sup>+</sup> mobility with increasing coordination number (up to 2.5); yet the fraction of mobile ions decreased. Thus, ligands dissociate Na<sup>+</sup> from larger ion clusters and aggregates, prescribe what the effective mass of Na<sup>+</sup> will be, and how Na<sup>+</sup> will move within the zwitterionic matrix via vehicular diffusion.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072521","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}
Hard carbon (HC) is a leading anode for sodium-ion batteries (SIBs), yet its practical application is hindered by Na plating stemming from its multistage Na-storage mechanism, which generates quasi-metallic Na clusters near the deposition potential, triggering uncontrolled metal deposition. Despite numerous advances in electrolyte design that improve cycling stability, the electrolyte dependence of Na plating is poorly understood. Herein, the Na plating behavior of HC in practical pouch-type full cells is systematically investigated, establishing electrolyte design principles that highlight the necessity of addressing Na plating/stripping reversibility alongside Na+ insertion/extraction. Na plating is found to be intrinsic and unavoidable under realistic operating conditions, including fast charging, prolonged cycling, and low-temperature cycling. Comparative analysis of ester-based (EC/DEC) and ether-based (G2) electrolytes reveals that the G2 electrolyte enables highly reversible Na plating/stripping, attributed to its lower desolvation barrier, faster interfacial kinetics, and the formation of an inorganic-rich solid electrolyte interphase (SEI). These findings underscore the importance of jointly enhancing the Na plating reversibility and SEI robustness for next-generation HC-based SIBs. Notably, ether-based formulations are validated as suitable for coupling low-voltage cathode systems, mitigating N/P ratio constraints, and unlocking higher energy densities.
{"title":"Mechanistic Insights into Sodium Plating in Hard Carbon Anodes: Electrolyte Design Principles for Practical Medium Voltage Sodium-Ion Full Batteries","authors":"Yuejing Zeng,Wei Li,Yuan Qin,Yang Yang,Jinbao Zhao","doi":"10.1021/acsenergylett.5c04116","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c04116","url":null,"abstract":"Hard carbon (HC) is a leading anode for sodium-ion batteries (SIBs), yet its practical application is hindered by Na plating stemming from its multistage Na-storage mechanism, which generates quasi-metallic Na clusters near the deposition potential, triggering uncontrolled metal deposition. Despite numerous advances in electrolyte design that improve cycling stability, the electrolyte dependence of Na plating is poorly understood. Herein, the Na plating behavior of HC in practical pouch-type full cells is systematically investigated, establishing electrolyte design principles that highlight the necessity of addressing Na plating/stripping reversibility alongside Na+ insertion/extraction. Na plating is found to be intrinsic and unavoidable under realistic operating conditions, including fast charging, prolonged cycling, and low-temperature cycling. Comparative analysis of ester-based (EC/DEC) and ether-based (G2) electrolytes reveals that the G2 electrolyte enables highly reversible Na plating/stripping, attributed to its lower desolvation barrier, faster interfacial kinetics, and the formation of an inorganic-rich solid electrolyte interphase (SEI). These findings underscore the importance of jointly enhancing the Na plating reversibility and SEI robustness for next-generation HC-based SIBs. Notably, ether-based formulations are validated as suitable for coupling low-voltage cathode systems, mitigating N/P ratio constraints, and unlocking higher energy densities.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"5 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097912","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}
Pub Date : 2026-01-29DOI: 10.1021/acsenergylett.5c03980
Dayoung Jun, Ju-Hyeon Lee, Se Hwan Park, Samick Son, Ji Hoon Lee, Yun Jung Lee
Mg particle-based “breathing” anodes provide a volumetrically adaptive host for all-solid-state batteries (ASSBs), yet structurally biased Li accumulation limits the long-term stability. Here, we demonstrate that the alloying mode of a secondary metal─solid-solution (Ag) versus intermetallic formation (Sn) decisively regulates Li-flux directionality and deposition pathways in Mg-based anodes. Ag dissolves continuously into the Li–Mg matrix, relaxing concentration gradients and redirecting Li growth toward the solid–electrolyte interface, which undermines the beneficial breathing behavior. In contrast, Sn forms immobile, stoichiometric Li22Sn5 domains that serve as internal nucleation anchors, guiding Li uniformly into the anode interior. As a result, the Sn-modified breathing anode exhibits markedly homogeneous volumetric expansion and significantly improves cycling stability, sustaining >500 cycles with an average Coulombic efficiency of 99.7% and 56.4% capacity retention, compared to about 350 cycles for pristine Mg. These results establish solid-solubility engineering as an effective strategy for enabling structurally resilient and volumetrically adaptive anode-free ASSBs.
{"title":"Alloy Phase-Formation-Driven Lithium Deposition Pathways in Magnesium-Based Breathing Anodes for Long-Lasting Anode-Free All-Solid-State Batteries","authors":"Dayoung Jun, Ju-Hyeon Lee, Se Hwan Park, Samick Son, Ji Hoon Lee, Yun Jung Lee","doi":"10.1021/acsenergylett.5c03980","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03980","url":null,"abstract":"Mg particle-based “breathing” anodes provide a volumetrically adaptive host for all-solid-state batteries (ASSBs), yet structurally biased Li accumulation limits the long-term stability. Here, we demonstrate that the alloying mode of a secondary metal─solid-solution (Ag) versus intermetallic formation (Sn) decisively regulates Li-flux directionality and deposition pathways in Mg-based anodes. Ag dissolves continuously into the Li–Mg matrix, relaxing concentration gradients and redirecting Li growth toward the solid–electrolyte interface, which undermines the beneficial breathing behavior. In contrast, Sn forms immobile, stoichiometric Li<sub>22</sub>Sn<sub>5</sub> domains that serve as internal nucleation anchors, guiding Li uniformly into the anode interior. As a result, the Sn-modified breathing anode exhibits markedly homogeneous volumetric expansion and significantly improves cycling stability, sustaining >500 cycles with an average Coulombic efficiency of 99.7% and 56.4% capacity retention, compared to about 350 cycles for pristine Mg. These results establish solid-solubility engineering as an effective strategy for enabling structurally resilient and volumetrically adaptive anode-free ASSBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"58 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072434","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}
Pub Date : 2026-01-29DOI: 10.1021/acsenergylett.5c03372
Yaelim Hwang, Shin-Yeong Kim, Haena Yim, Sang-Hwan Oh, Ji Hyun Lee, Yeseul Kim, Yunseo Jeoun, So Hee Kim, Jae-Hong Lim, Byung Mook Weon, Ho Won Jang, Seung-Ho Yu, Yung-Eun Sung, Ji-Won Choi
Anode-free all-solid-state batteries (AFASSBs) have emerged as promising candidates for next-generation energy storage systems due to their high safety and potential for exceptionally high gravimetric and volumetric energy densities. However, achieving long-term cycling stability remains a critical challenge because of nonuniform Li plating/stripping. A dual-component, bifunctional interfacial coating at the current collector/solid electrolyte interface, incorporating both a protective layer and seed sites, is considered critical for uniform Li plating and formation of a stable interface. Nevertheless, how the dual-component redistribution changes during cycling remains poorly understood, and design guidelines for effectively harnessing this phenomenon are still lacking. Here, we employ a gradient cosputtering approach to produce dual-element coated current collectors in which Ag serves as a Li-affinitive nucleation seed and Si functions as an ion-conducting protective interlayer. Compositional gradients enabled a systematic study of composition-dependent behaviors, and ex-situ analyses revealed that a lower Si fraction in the protective layer promotes a “reversible redistribution”, where Si repeatedly migrate during cycling, preventing crack formation over prolonged cycling. The optimized Ag with 1 mol % Si electrode achieved stable cycling even at room temperature. This bifunctional interfacial design provides valuable mechanistic insights and practical guidelines for engineering dual-component electrode architectures for stable, high-energy-density AFASSBs.
{"title":"Reversible Redistribution in Ag–Si Electrodes for Stable Anode-Free All-Solid-State Batteries","authors":"Yaelim Hwang, Shin-Yeong Kim, Haena Yim, Sang-Hwan Oh, Ji Hyun Lee, Yeseul Kim, Yunseo Jeoun, So Hee Kim, Jae-Hong Lim, Byung Mook Weon, Ho Won Jang, Seung-Ho Yu, Yung-Eun Sung, Ji-Won Choi","doi":"10.1021/acsenergylett.5c03372","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03372","url":null,"abstract":"Anode-free all-solid-state batteries (AFASSBs) have emerged as promising candidates for next-generation energy storage systems due to their high safety and potential for exceptionally high gravimetric and volumetric energy densities. However, achieving long-term cycling stability remains a critical challenge because of nonuniform Li plating/stripping. A dual-component, bifunctional interfacial coating at the current collector/solid electrolyte interface, incorporating both a protective layer and seed sites, is considered critical for uniform Li plating and formation of a stable interface. Nevertheless, how the dual-component redistribution changes during cycling remains poorly understood, and design guidelines for effectively harnessing this phenomenon are still lacking. Here, we employ a gradient cosputtering approach to produce dual-element coated current collectors in which Ag serves as a Li-affinitive nucleation seed and Si functions as an ion-conducting protective interlayer. Compositional gradients enabled a systematic study of composition-dependent behaviors, and <i>ex-situ</i> analyses revealed that a lower Si fraction in the protective layer promotes a “reversible redistribution”, where Si repeatedly migrate during cycling, preventing crack formation over prolonged cycling. The optimized Ag with 1 mol % Si electrode achieved stable cycling even at room temperature. This bifunctional interfacial design provides valuable mechanistic insights and practical guidelines for engineering dual-component electrode architectures for stable, high-energy-density AFASSBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"140 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097856","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}
Pub Date : 2026-01-28DOI: 10.1021/acsenergylett.5c03228
Jianing Duan, Junke Jiang, Unsoo Kim, Jong Woo Lee, Yingguo Yang, Mansoo Choi, Zhaoxin Wu, Jun Xi
Despite the attractive properties of two-dimensional (2D) perovskites, the structural origin of their photostability remains elusive, especially extending to device scales. This work systematically investigates spacer engineering in quasi-2D single crystals (n = 2) using para-substituted phenylethylamine derivatives (XPEA), establishing critical correlations between the spacer conformation and the structural/electronic properties of hybrid lattices. We find that the BrPEA cation is conducive to strengthening the organic–inorganic interface and suppressing the structural fluctuations of the inorganic framework, thereby stabilizing the overall lattice. Integrated experiments and simulations confirm the optimal photostability of the BrPEA-based lattice. In photovoltaic devices, BrPEA promotes optimized film morphology, homogeneous phase distribution, and improved charge-carrier dynamics, yielding a high device efficiency. Operational stability analysis reveals that device degradation is initially governed by spacer-related structural robustness, while photoactivated trap states dominate at excessive defect densities. This work provides a guideline for engineering organic spacers to enhance 2D perovskite photostability for cutting-edge optoelectronic applications.
{"title":"Structure and Device-Operando Photostability of Quasi-2D Ruddlesden–Popper Perovskites: Engineering the Spacer Cation Matters","authors":"Jianing Duan, Junke Jiang, Unsoo Kim, Jong Woo Lee, Yingguo Yang, Mansoo Choi, Zhaoxin Wu, Jun Xi","doi":"10.1021/acsenergylett.5c03228","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03228","url":null,"abstract":"Despite the attractive properties of two-dimensional (2D) perovskites, the structural origin of their photostability remains elusive, especially extending to device scales. This work systematically investigates spacer engineering in quasi-2D single crystals (<i>n</i> = 2) using para-substituted phenylethylamine derivatives (XPEA), establishing critical correlations between the spacer conformation and the structural/electronic properties of hybrid lattices. We find that the BrPEA cation is conducive to strengthening the organic–inorganic interface and suppressing the structural fluctuations of the inorganic framework, thereby stabilizing the overall lattice. Integrated experiments and simulations confirm the optimal photostability of the BrPEA-based lattice. In photovoltaic devices, BrPEA promotes optimized film morphology, homogeneous phase distribution, and improved charge-carrier dynamics, yielding a high device efficiency. Operational stability analysis reveals that device degradation is initially governed by spacer-related structural robustness, while photoactivated trap states dominate at excessive defect densities. This work provides a guideline for engineering organic spacers to enhance 2D perovskite photostability for cutting-edge optoelectronic applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"73 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146057131","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}
Pub Date : 2026-01-28DOI: 10.1021/acsenergylett.5c03292
Wonil Jung, Jeehoon Shin, Thomas E. Mallouk
Inorganic solid-state hydroxide ion conductors have emerged as stable platforms for high-temperature alkaline energy conversion technologies. Although several materials have shown promising ionic conductivity in model studies, their direct implementation in operating devices has remained largely unexplored. Here, we demonstrate that silver(I) oxide (Ag2O) nanoparticles can function as hydroxide ion conductors within anion exchange membrane fuel cells (AEMFCs). Syringe-filtered 1–6 nm Ag2O nanoparticles were integrated into Pt/C cathodes, establishing ionic conduction pathways across the cathode–membrane interface. The resulting ionomer-free membrane electrode assembly (MEA) achieved 1.91 W cm–2 peak power density at 2.4 wt % Ag2O loading and maintained stable mass transport during 100 h of continuous operation at 0.6 A cm–2. Electrochemical and structural analyses revealed how Ag2O loading influences ionic conduction, pore structure, and mass transport behavior in ways that are partially distinct from conventional ionomer-based electrodes. These findings highlight inorganic solid-state conductors as promising design analogues to ionomers for high-performance, ionomer-free AEMFC cathodes.
无机固体氢氧离子导体已成为高温碱性能量转换技术的稳定平台。虽然有几种材料在模型研究中显示出有希望的离子电导率，但它们在操作设备中的直接应用在很大程度上仍未被探索。在这里，我们证明了氧化银（Ag2O）纳米颗粒可以作为氢氧离子导体在阴离子交换膜燃料电池（aemfc）中发挥作用。经注射器过滤的1-6 nm Ag2O纳米颗粒被整合到Pt/C阴极中，在阴极-膜界面上建立了离子传导途径。所得到的无离聚体膜电极组件（MEA）在2.4 wt % Ag2O负载下达到1.91 W cm-2的峰值功率密度，并在0.6 A cm-2的连续运行100小时内保持稳定的质量传输。电化学和结构分析揭示了Ag2O负载如何影响离子传导、孔隙结构和质量传递行为，其方式部分不同于传统的基于离子单体的电极。这些发现突出了无机固态导体作为高性能、无离聚体AEMFC阴极的有前途的设计类似物。
{"title":"Silver Oxide Nanoparticles as Solid-State Hydroxide Ion Conductors for Watt-Scale Anion Exchange Membrane Fuel Cells","authors":"Wonil Jung, Jeehoon Shin, Thomas E. Mallouk","doi":"10.1021/acsenergylett.5c03292","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03292","url":null,"abstract":"Inorganic solid-state hydroxide ion conductors have emerged as stable platforms for high-temperature alkaline energy conversion technologies. Although several materials have shown promising ionic conductivity in model studies, their direct implementation in operating devices has remained largely unexplored. Here, we demonstrate that silver(I) oxide (Ag<sub>2</sub>O) nanoparticles can function as hydroxide ion conductors within anion exchange membrane fuel cells (AEMFCs). Syringe-filtered 1–6 nm Ag<sub>2</sub>O nanoparticles were integrated into Pt/C cathodes, establishing ionic conduction pathways across the cathode–membrane interface. The resulting ionomer-free membrane electrode assembly (MEA) achieved 1.91 W cm<sup>–2</sup> peak power density at 2.4 wt % Ag<sub>2</sub>O loading and maintained stable mass transport during 100 h of continuous operation at 0.6 A cm<sup>–2</sup>. Electrochemical and structural analyses revealed how Ag<sub>2</sub>O loading influences ionic conduction, pore structure, and mass transport behavior in ways that are partially distinct from conventional ionomer-based electrodes. These findings highlight inorganic solid-state conductors as promising design analogues to ionomers for high-performance, ionomer-free AEMFC cathodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"80 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146097858","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}
Pub Date : 2026-01-28DOI: 10.1021/acsenergylett.5c03360
Qikai Shentu, Binbin Pan, Kewen Xing, Keliang Li, Na Han, Yanguang Li
Electrochemical valorization of small molecules such as H2O, CO2, and N2 into value-added products represents a sustainable strategy to mitigate greenhouse gas emissions and store intermittent renewable energy in high-energy-density chemicals. Traditionally, these processes couple with the water oxidation reaction at the anode, which unfortunately suffers from high overpotentials and thus limits the overall energy efficiency. Over the past decade, alternative anodic reactions have been explored to improve energy efficiency and enhance the product value. Despite their potential, significant technical challenges remain before practical implementation can be realized. In this Perspective, we briefly overview the current status of coupling alternative anodic reactions for the electrochemical valorization of small molecules and discuss the key challenges and potential solutions from the viewpoints of catalyst design, electrolyzer engineering, and product separation. We aim to highlight how these advances collectively pave the way toward more energy-efficient, economically viable, and sustainable electrochemical manufacturing.
{"title":"Coupling Alternative Anodic Reactions in Electrochemical Valorization","authors":"Qikai Shentu, Binbin Pan, Kewen Xing, Keliang Li, Na Han, Yanguang Li","doi":"10.1021/acsenergylett.5c03360","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03360","url":null,"abstract":"Electrochemical valorization of small molecules such as H<sub>2</sub>O, CO<sub>2</sub>, and N<sub>2</sub> into value-added products represents a sustainable strategy to mitigate greenhouse gas emissions and store intermittent renewable energy in high-energy-density chemicals. Traditionally, these processes couple with the water oxidation reaction at the anode, which unfortunately suffers from high overpotentials and thus limits the overall energy efficiency. Over the past decade, alternative anodic reactions have been explored to improve energy efficiency and enhance the product value. Despite their potential, significant technical challenges remain before practical implementation can be realized. In this Perspective, we briefly overview the current status of coupling alternative anodic reactions for the electrochemical valorization of small molecules and discuss the key challenges and potential solutions from the viewpoints of catalyst design, electrolyzer engineering, and product separation. We aim to highlight how these advances collectively pave the way toward more energy-efficient, economically viable, and sustainable electrochemical manufacturing.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"22 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146057132","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sodium-ion batteries (SIBs) are applied for large-scale energy storage systems, yet their energy density remains capped by hard carbon (HC) anodes with modest gravimetric and volumetric capacities. Herein, we report an alloying-carbon strategy that applies microsized Sn particles with microsized HC particles to form thick-film anodes. The optimized Sn-HC composite couples the high capacity and compaction density of Sn with the structural robustness of HC, displaying the gravimetric and volumetric capacities of 583 mAh g–1 and 1073 mAh cm–3, an initial Coulombic efficiency of 90.5%, a capacity retention of ∼89.5% after 1000 cycles at 0.5 A g–1, and limited electrode swelling of 33.7%. Coupled with the Na3V2(PO4)3 cathode, the SIB full cell delivers an energy density of 254 Wh kg–1 and high-rate capabilities. Such Sn-HC architecture offers a scalable and industrially relevant route to simultaneously increase the gravimetric and volumetric capacities of anodes for SIBs.
钠离子电池（sib）应用于大规模储能系统，但其能量密度仍然受到硬碳（HC）阳极的限制，其重量和体积容量适中。在此，我们报告了一种合金化碳策略，将微Sn颗粒与微HC颗粒结合形成厚膜阳极。优化后的Sn-HC复合材料将Sn的高容量和高压实密度与HC的结构坚固性结合在一起，其重量和体积容量分别为583 mAh g-1和1073 mAh cm-3，初始库仑效率为90.5%，在0.5 a g-1下循环1000次后容量保留率为~ 89.5%，电极膨胀限制为33.7%。与Na3V2(PO4)3阴极相结合，SIB全电池提供了254 Wh kg-1的能量密度和高速率能力。这种Sn-HC架构提供了一种可扩展的和工业相关的路线，同时增加sib阳极的重量和体积容量。
{"title":"Microsized Sn-Hard Carbon Composite Anode with Capacities of 583 mAh g–1 and 1073 mAh cm–3 for Sodium-Ion Batteries","authors":"Xiang Gao, Zerui Yan, Lixin Lin, Huilong Liu, Yuting Song, Jiawei Guo, Yi Gong, Jianming Tao, Jiaxin Li, Guoqiang Zou, Yingbin Lin, Yunlong Zhao, Dong-liang Peng, Qiulong Wei","doi":"10.1021/acsenergylett.5c03621","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c03621","url":null,"abstract":"Sodium-ion batteries (SIBs) are applied for large-scale energy storage systems, yet their energy density remains capped by hard carbon (HC) anodes with modest gravimetric and volumetric capacities. Herein, we report an alloying-carbon strategy that applies microsized Sn particles with microsized HC particles to form thick-film anodes. The optimized Sn-HC composite couples the high capacity and compaction density of Sn with the structural robustness of HC, displaying the gravimetric and volumetric capacities of 583 mAh g<sup>–1</sup> and 1073 mAh cm<sup>–3</sup>, an initial Coulombic efficiency of 90.5%, a capacity retention of ∼89.5% after 1000 cycles at 0.5 A g<sup>–1</sup>, and limited electrode swelling of 33.7%. Coupled with the Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode, the SIB full cell delivers an energy density of 254 Wh kg<sup>–1</sup> and high-rate capabilities. Such Sn-HC architecture offers a scalable and industrially relevant route to simultaneously increase the gravimetric and volumetric capacities of anodes for SIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"221 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2026-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072523","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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