Wei Zhang, Adnan Ozden, Yu Yang, Aoni Xu, Fengwang Li
{"title":"Hidden Acidification Challenges in Electrochemical Ocean Decarbonization","authors":"Wei Zhang, Adnan Ozden, Yu Yang, Aoni Xu, Fengwang Li","doi":"10.1021/acsenergylett.5c00900","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00900","url":null,"abstract":"Electrochemical direct ocean capture (eDOC) is an emerging methodology for carbon capture. However, our comprehensive thermodynamic and initial kinetic analyses reveal critical challenges inherent in the electrochemical pH-swing process. Specifically, the mixture of treated ocean water post-eDOC fails to achieve complete neutralization, resulting in unintended ocean acidification. This issue stems from the disproportionate impacts of acidification and alkalinization on dissolved inorganic carbon dynamics and hydroxide precipitation. Our findings underscore the necessity for innovative process designs that effectively balance pH shifts and manage precipitate formation, thereby ensuring the environmental sustainability of eDOC technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"53 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143979873","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}
{"title":"Visualizing Electron Transport and Interface Evolution of Li3InCl6-Based Composite Cathode for All-Solid-State Batteries","authors":"Rui Li, Yanpei Fan, Xiaotong Liu, Jiewen Li, Haodong Zhang, Lin Lin, Zhenbin Wang, Bohua Wen","doi":"10.1021/acsenergylett.5c00174","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00174","url":null,"abstract":"All-solid-state batteries (ASSBs) promise higher energy density and improved safety, but stable solid electrolyte-electrode interfaces remain a key challenge. Mixed ionic-electronic conducting interphases cause degradation, limiting the cathode lifetime. Here, we employ <i>operando</i> electrochemical atomic force microscopy based on modified Kelvin probe force microscopy to visualize nanoscale electron transport and dynamic evolution of the composite cathode interface. By analyzing the contact current (<i>I</i><sub>c</sub>) distribution, we distinguish the interfacial stability of Li<sub>3</sub>InCl<sub>6</sub> (LIC)-based cathodes with LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub>, both coated and uncoated with LiNbO<sub>3</sub>, and conductive carbon additives. <i>Operando</i> studies, combined with interfacial mechanical property mapping, reveal that the <i>I</i><sub>c</sub> heterogeneity and magnitude critically influence degradation. In LIC-based cathodes, decomposed organic interphases enhance electron transport, driving the formation of high-modulus inorganic species that accelerate LIC breakdown. These findings link microscopic electron transport and interface evolution to electrochemical performance, offering insights for designing stable interphases to advance ASSB technology.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066441","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}
Yang He, Sheng Gao, Bo Zhao, Huiwen Chen, Ziyao Zhu, Mingrui Yu, Yang Zhang, Yang Li, Martin Stolterfoht, Xueqing Yang, Xingzhu Wang, Yunlong Li
{"title":"Epitaxial Growth of High-Quality Perovskite Heterojunctions for Direct-Conversion X-ray Detectors","authors":"Yang He, Sheng Gao, Bo Zhao, Huiwen Chen, Ziyao Zhu, Mingrui Yu, Yang Zhang, Yang Li, Martin Stolterfoht, Xueqing Yang, Xingzhu Wang, Yunlong Li","doi":"10.1021/acsenergylett.5c00938","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00938","url":null,"abstract":"Three-dimensional metal halide perovskites (3D-MHPs) have emerged as potential semiconductors for direct-conversion X-ray detectors. However, excessive ion migration in 3D-MHPs compromises device stability, hindering practical deployment. While perovskite heterojunctions have been explored to suppress ion migration, their effectiveness are often limited by challenges in fabricating high-quality heterojunctions, resulting in suboptimal charge collection compared to individual perovskite crystals. In this work, a liquid-phase interfacial array-epitaxial growth method was developed to construct high-quality MAPbBr<sub>3</sub>/MAPbI<sub>3</sub> heterojunctions for direct X-ray detectors. The heterojunction crystal exhibit a serrated, ultrathick transition region that enhances X-ray response by increasing the interfacial contact area between MAPbBr<sub>3</sub> and MAPbI<sub>3</sub>. Consequently, the fabricated detectors demonstrate stable operational performance, a high sensitivity of 0.99 × 10<sup>6</sup> μC Gy<sub>air</sub><sup>–1</sup> cm<sup>–2</sup>, and an ultralow detection limit of 0.56 nGy<sub>air</sub> s<sup>–1</sup>. Furthermore, the built-in electric field enables self-powered X-ray detection at 0 V bias, achieving a sensitivity of 1.16 × 10<sup>3</sup> μC Gy<sub>air</sub><sup>–1</sup> cm<sup>–2</sup>.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"8 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143979874","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}
{"title":"Phase Evolution Extension of Cu2ZnSn(S,Se)4 Absorber Boosting the Efficiency of Kesterite Solar Cells to 14.99%","authors":"Ge Yao, Zucheng Wu, Dongxing Kou, Bingyin Kong, Hao Wei, Zhipeng Shao, Wenhui Zhou, Zhengji Zhou, Shengjie Yuan, Yafang Qi, Litao Han, Guanglei Cui, Sixin Wu","doi":"10.1021/acsenergylett.5c01007","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01007","url":null,"abstract":"The presence of secondary phases and a high concentration of deep-level defects led to a large open-circuit voltage deficit (V<sub>oc,deficit</sub>) for Cu<sub>2</sub>ZnSn(S,Se)<sub>4</sub> (CZTSSe) solar cells. Here we regulate the phase evolution from CZTS to CZTSSe in the initial selenization stage to obtain high-quality absorber with minimal defects and secondary phases. By adding the bidentate chelation structured mercaptopropionic acid (MPA) into the air-prepared 2-methoxyethanol (MOE) precursor solution, large CZTS colloidal particles and dense precursor films are prepared. During the initial selenization stage, the reduced nucleation sites can decrease selenium–molecule interactions and extend the phase evolution process. This extension makes the heterogeneous nucleation more controllable, fostering uniform element distribution and enhanced growth of <i>permeating the large-grain layer</i>. These benefits demonstrate a substantial increase in device efficiency up to 14.99% (certified at 14.38%) with a reduced V<sub>oc,deficit</sub> of 281.18 mV. The findings are of great significance for further efficiency leaps of kesterite solar cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"122 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143945621","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}
Tino Lukas, Seongrok Seo, Philippe Holzhey, Katherine Stewart, Charlie Henderson, Lukas Wagner, David Beynon, Trystan M. Watson, Ji-Seon Kim, Markus Kohlstädt, Henry J. Snaith
{"title":"Charge Extraction Multilayers Enable Positive-Intrinsic-Negative Perovskite Solar Cells with Carbon Electrodes","authors":"Tino Lukas, Seongrok Seo, Philippe Holzhey, Katherine Stewart, Charlie Henderson, Lukas Wagner, David Beynon, Trystan M. Watson, Ji-Seon Kim, Markus Kohlstädt, Henry J. Snaith","doi":"10.1021/acsenergylett.4c03403","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03403","url":null,"abstract":"Perovskite solar cells achieve high power conversion efficiencies but usually rely on vacuum-deposited metallic contacts, leading to high material costs for noble metals and stability issues for more reactive metals. Carbon-based materials offer a cost-effective and potentially more stable alternative. The vast majority of carbon-electrode PSCs use the negative-intrinsic-positive (n-i-p) or “hole-transport-layer-free” architectures. Here, we present a systematic study to assess the compatibility of “inverted”, p-i-n configuration PSC contact layers with carbon top electrodes. We identify incompatibilities between common electron transport layers and the carbon electrode deposition process and previously unobserved semiconducting properties in carbon electrodes with unique implications for charge extraction and electronic behavior. To overcome these issues, we introduce a double-layer atomic layer deposited tin oxide (SnO<sub>2</sub>) and Poly(2,3-dihydrothieno-1,4-dioxin)-poly(styrenesulfonate) (PEDOT:PSS), yielding up to 16.1% PCE and a retained 94% performance after 500 h of outdoor aging. The study is a crucial step forward for printable, metal-electrode-free, and evaporation-free perovskite PV technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"55 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940064","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}
{"title":"Multiscale Structure Regulation Induced by Fluorine Coordination Enables High-Performance and Durable PEMFC","authors":"Jingsen Bai, Xin Guan, Hanshi Qu, Liang Liang, Chunyu Ru, Xue Gong, Zhao Jin, Meiling Xiao, Changpeng Liu, Wei Xing","doi":"10.1021/acsenergylett.5c00510","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00510","url":null,"abstract":"The stability enhancement of metal–nitrogen–carbon (M–N–C) is often inevitably accompanied by a loss of activity. Additionally, during the long-term operation, the activity frequently declines due to water flooding effects, significantly reducing the lifetime of the membrane electrode assembly (MEA). Herein, fluorine (F)-doping was employed to bypass the activity–stability trade-off of Fe–N–C catalysts. F incorporation increases the metal dissolution energy and lowers the electron density of Fe–N<sub>4</sub> sites, improving both stability and catalytic activity. Besides, the hydrophobicity of F can improve water management performance within the MEA, markedly reducing oxygen transport resistance. As a result, the F-doped Fe–N–C cathode enables a high peak power density of 1.1 W cm<sup>–2</sup>, far exceeding the Fe–N–C counterpart (0.79 W cm<sup>–2</sup>). More importantly, 90% of the power density can be retained after 30000 cycles of accelerated stress testing, demonstrating huge application potential in fuel cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"57 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940114","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}
Jun Beom Kim, Jaewon Baek, Balamurugan Jayaraman, Sujin Cha, Gang San Lee, Yeo Hoon Yoon, Go Bong Choi, Colin Wing-Lok Cheng, Joonwon Lim, Hee-Tak Kim, Sang Ouk Kim
{"title":"Two-Step Graphene Strategy Enabling Long-Cycle Stability of Silicon Anodes","authors":"Jun Beom Kim, Jaewon Baek, Balamurugan Jayaraman, Sujin Cha, Gang San Lee, Yeo Hoon Yoon, Go Bong Choi, Colin Wing-Lok Cheng, Joonwon Lim, Hee-Tak Kim, Sang Ouk Kim","doi":"10.1021/acsenergylett.5c01032","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01032","url":null,"abstract":"A two-step graphene-reinforced hierarchical structure to address the poor cycle stability due to significant volume fluctuations in silicon anodes for lithium-ion batteries (LIBs) is introduced in this study. Fine composite granules (1–2 μm), SiNPs@rGO where silicon nanoparticles (SiNPs) were fully encapsulated by reduced graphene oxide (rGO) flakes, were synthesized by a high-power planetary ball milling technique. The compact structure of the SiNPs@rGO granules effectively suppressed the dispersion loss of Si and Li<sub><i>x</i></sub>Si fragments from the granules. To accommodate the large volume fluctuation of Si in lithiation and delithiation cycles, a hierarchical structure using mechanically flexible and stretchable holey reduced graphene oxide (HrGO) 2D layers was developed. The hierarchical structure of HrGO/SiNPs@rGO composite anode successfully accommodated the volume fluctuations of SiNPs@rGO, thereby markedly enhancing long-cycle stability. Systematic analyses of the characteristic electrochemical properties and morphological evolution of these 2D material-based anodes are reported.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"28 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933397","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}
Austin G. Kuba, Florent Sahli, Mostafa Othman, Kerem Artuk, Quentin Jeangros, Aïcha Hessler-Wyser, Christophe Ballif, Christian M. Wolff
{"title":"Making from Breaking: Degradation Inversion Enables Vapor-Phase Synthesis of Halide Perovskites in Ambient Conditions","authors":"Austin G. Kuba, Florent Sahli, Mostafa Othman, Kerem Artuk, Quentin Jeangros, Aïcha Hessler-Wyser, Christophe Ballif, Christian M. Wolff","doi":"10.1021/acsenergylett.4c03395","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03395","url":null,"abstract":"Vapor phase deposition of formamidinium-rich perovskites is hampered by the decomposition of formamidine in the vapor phase. We use the reversibility of this reaction to establish a dynamic equilibrium that enables the vapor-phase synthesis of formamidinium iodide from the “degradation products” s-triazine, ammonia, and hydrogen iodide and thereby convert lead halide thin films to lead halide perovskites. Finally, we produce the first proof of concept solar cells via this innovative process.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"67 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933395","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}
{"title":"Origin of Solid Electrolyte Interphase Heterogeneity on Lithium Metal Anodes and Its Mitigation with Electrolyte Additives","authors":"Aoxuan Wang, Ting Yang, Linxue Zhang, Changdong Li, Hao Chen, Yumeng Zhao, Jiayan Luo","doi":"10.1021/acsenergylett.5c00594","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00594","url":null,"abstract":"Lithium metal anode (LMA) stands as a promising candidate for next-generation high-energy-density batteries, yet its viability is critically compromised by heterogeneous solid electrolyte interphase (SEI) formation. This interfacial inhomogeneity manifested as spatially fluctuating Li<sup>+</sup> transport kinetics provokes erratic lithium deposition and dendrite propagation. Here, we reveal that current strategies to homogenize SEI are impeded by an overlooked origin: crystallographic anisotropy-driven adsorption bias of electrolyte components across polycrystalline Li (poly-Li) surfaces, thereby dictating SEI heterogeneity. We further decouple the correlation between lattice orientation and adsorption energetics by engineering a dual-additive electrolyte [fluoroethylene carbonate (FEC) and propane sultone (PS)]. These additives establish plane adsorption uniformity, forming a homogeneous SEI that spatially synchronizes Li<sup>+</sup> flux. When paired with a high-loading LiCoO<sub>2</sub> cathode (3.86 mAh cm<sup>–2</sup>), the stabilized anode enables 80% capacity retention over 380 cycles under ultralean conditions (N/P = 2.30, E/C = 2.34 g Ah<sup>–1</sup>), tripling the cycle life versus conventional electrolytes while suppressing dendritic failure modes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"112 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143940110","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}
{"title":"Unexpected Planar Gliding and Microcracking Induced by Neutron Irradiation in Single-Crystalline LiCoO2 Cathodes","authors":"Kang Wu, Lihua Mo, Tiancheng Yi, Zhigang Zhang, Yoshihiro Kuroiwa, Sangwook Kim, Peilin Ran, Wen Yin, Fangwei Wang, Quanzhi Yu, Tianjiao Liang, Jinkui Zhao, Enyue Zhao","doi":"10.1021/acsenergylett.5c00828","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00828","url":null,"abstract":"Lithium-ion batteries have become increasingly vital in powering aerospace applications, where radiation resistance is a mission-critical battery property. Little is known about the effects of space irradiation on battery materials in operation, particularly neutron irradiation. Understanding the structural and electrochemical failure mechanisms of battery materials in radiation environments is thus crucial for high-performance aerospace applications. Here, we investigate LiCoO<sub>2</sub> (LCO) cathode degradation under simulated space radiation at the China Spallation Neutron Source. Broad-spectrum neutron exposure (ranging from meV to GeV) induces microcracks and stress in LCO crystals, impairing Li<sup>+</sup> diffusion and destabilizing the oxygen framework. <i>Operando</i> neutron studies reveal that capacity loss stems from irradiation-triggered interlayer planar gliding during Li de/intercalation. Finally, we show that the irradiation damage can be effectively mitigated by reducing the LCO crystalline particle size. Thus, our work provides the critical knowledge for designing radiation-resistant cathode materials for critical applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"5 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143933399","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}