Dongqin Yuan, Yangyu Liu, Jing Xu, Wenxiao Niu, Xingjiao Feng, Heyong Wang, Pengpeng Teng, Jie Yang, Tao Yu, Zhigang Zou, Chunxiong Bao
{"title":"Decoupling the Roles of Mobility and Energy Level of Hole-Transport Layers to Efficiency Roll-Off in Perovskite Light-Emitting Diodes","authors":"Dongqin Yuan, Yangyu Liu, Jing Xu, Wenxiao Niu, Xingjiao Feng, Heyong Wang, Pengpeng Teng, Jie Yang, Tao Yu, Zhigang Zou, Chunxiong Bao","doi":"10.1021/acsenergylett.5c01169","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01169","url":null,"abstract":"Metal halide perovskite light-emitting diodes (PeLEDs) have attracted significant attention due to their high efficiency, low cost, and solution processability. While the peak efficiency of PeLEDs has been significantly enhanced, severe efficiency roll-off remains a critical challenge for bright and stable devices. In this study, we investigate the impact of the hole transport layer (HTL) to the efficiency roll-off in PeLED based on FAPbI<sub>3</sub>. Our findings reveal that the hole mobility of the HTL plays a crucial role in mitigating efficiency roll-off of the device, whereas the energy-level alignment primarily governs the peak efficiency. Furthermore, we implement an HTL with high hole mobility and proper energy-level alignment to promote charge carrier balance, thereby simultaneously realizing peak external quantum efficiency (EQE) enhancement and mitigating efficiency roll-off in FAPbI<sub>3</sub>-based PeLEDs. Compared with near-infrared devices using the widely adopted low-mobility random copolymer HTL, our devices deliver a peak EQE of 21.7% at 84 mA cm<sup>–2</sup>, retain over 10% EQE at 1300 mA cm<sup>–2</sup>, and exhibit nearly 5-fold higher radiance. This study highlights the distinct roles of hole mobility and energy-level alignment in governing efficiency roll-off and peak device efficiency.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"25 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144520921","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":"In Situ Engineering of a Multifunctional Cathode–Electrolyte Interphase for Advanced Sodium-Ion Batteries","authors":"Chunye Yang, Jiaxuan Wang, Chunchun Sang, Wanhao Zheng, Hansong Cui, Xinping Ai, Yuliang Cao, Yongjin Fang","doi":"10.1021/acsenergylett.5c01335","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01335","url":null,"abstract":"Layered transition metal oxides have been considered promising cathode candidates for sodium-ion batteries due to their exceptional specific capacity and tunable composition. Nevertheless, their commercialization faces critical challenges, including irreversible phase transitions, hygroscopic degradation, and thermal runaway risks. To address these limitations, we propose a strategy for the <i>in situ</i> construction of an artificial cathode–electrolyte interphase (CEI) layer, which facilitates rapid Na<sup>+</sup> diffusion kinetics and suppresses detrimental interfacial side reactions. The modified Na<sub>2/3</sub>Ni<sub>1/3</sub>Mn<sub>2/3</sub>O<sub>2</sub> electrode delivers a remarkable reversible capacity of 150 mAh g<sup>–1</sup> at 0.1 C while maintaining 84% capacity retention over 200 cycles at 1 C (vs 67% for pristine). Notably, the CEI-modified cathode exhibits significant air tolerance, retaining 96% of initial capacity after 7-day ambient exposure. Furthermore, thermal analysis confirms enhanced thermal stability of the battery, effectively mitigating safety concerns. The work establishes a universal paradigm for stabilizing electrode materials, providing critical insights for developing robust sodium-ion battery systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"8 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144521086","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}
Michael A. Baird, Ryan S. Kingsbury, Yunfei Wang, Chenhui Zhu, Gan Chen, Liana Klivansky, Michael L. Whittaker, Brett A. Helms
{"title":"Electrochemical Li+ Enrichment of Mixed-Cation Brines with Antiselective Polymer Membranes","authors":"Michael A. Baird, Ryan S. Kingsbury, Yunfei Wang, Chenhui Zhu, Gan Chen, Liana Klivansky, Michael L. Whittaker, Brett A. Helms","doi":"10.1021/acsenergylett.5c01120","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01120","url":null,"abstract":"Natural brines with dilute quantities of Li<sup>+</sup> are attractive as feedstocks for battery electric vehicle supply chains because of their onshore abundance. Electrolytic membrane reactors employing Li<sup>+</sup>-antiselective membranes are ideal for continuous removal of Na<sup>+</sup> and other metals, upgrading brine quality and value. Here, we show that the selectivity of microporous polymer membranes and the permeability of cation exchange membranes can be combined in sulfonated polymers of intrinsic microporosity to defy conventional selectivity–permeability trade-offs for mixed-cation separations. The concentration-normalized Na<sup>+</sup>/Li<sup>+</sup> selectivity reaches 3.03 due to mixed-ion effects, enabling the removal of 29% of Na<sup>+</sup> ions and 41% of K<sup>+</sup> ions from a brine sample from Teel’s Marsh (NV, USA) in less than 1 h, while only extracting 9.5% of Li<sup>+</sup>, producing a Li-enriched effluent. We discuss these results in the context of electrochemical efficiency, offering design criteria for minimizing losses originating from competing transport processes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"3 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144533756","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}
Changlin Zhou, Julie Descamps, Bertrand Goudeau, Patrick Garrigue, Frédéric Bedu, Lionel Santinacci, Zonghua Wang, Neso Sojic, Gabriel Loget
{"title":"Photoelectrochemical Charge Transfer Imaging at Nanoscale Catalysts","authors":"Changlin Zhou, Julie Descamps, Bertrand Goudeau, Patrick Garrigue, Frédéric Bedu, Lionel Santinacci, Zonghua Wang, Neso Sojic, Gabriel Loget","doi":"10.1021/acsenergylett.5c01296","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01296","url":null,"abstract":"Semiconductor (SC)-based photoelectrodes, employed for the production of solar fuels, such as H<sub>2</sub> or small organic molecules, have garnered significant attention and extensive studies because they could play a crucial role in addressing the global energy crisis. While macroscopic photoelectrochemical (PEC) studies of these systems are routinely employed to monitor the overall activity of these systems, the spatiotemporal resolution of local PEC activity down to the nanoscale remains a challenge, which could lead to considerable improvement in photoelectrode design and engineering. Here, model Si-based photoanodes precisely coated with water-splitting Ni catalysts of various sizes are studied by photoinduced electrochemiluminescence (PECL) microscopy. Our results demonstrate that this method allows precise imaging of hole-driven photoelectrochemical reactivity down to a scale of ∼50 nm, making PECL microscopy a valuable tool for elucidating charge transfer and local interfacial activity of photoelectrodes employed in PEC solar energy conversion processes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"36 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144521113","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}
Jingya Xin, Jingfan Shao, Xiaohan Yu, Wei Huang, Yanguang Li
{"title":"Deciphering the Controversial Role of Sacrificial Agents in Photocatalytic H2O2 Production: Promoters or Source of Artifacts?","authors":"Jingya Xin, Jingfan Shao, Xiaohan Yu, Wei Huang, Yanguang Li","doi":"10.1021/acsenergylett.5c01771","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01771","url":null,"abstract":"Photocatalytic H<sub>2</sub>O<sub>2</sub> synthesis holds great promise for sustainable H<sub>2</sub>O<sub>2</sub> production. While extensive efforts have focused on optimizing catalysts and reaction conditions to enhance H<sub>2</sub>O<sub>2</sub> yields, the accuracy of H<sub>2</sub>O<sub>2</sub> quantification─a fundamental prerequisite for reliable performance evaluation─remains underexplored. Conventional colorimetric methods can be compromised by the widespread use of organic sacrificial agents due to their intrinsic redox activity and optical absorption properties. Herein, we systematically investigate the interference effects of common sacrificial agents and their oxidation products on H<sub>2</sub>O<sub>2</sub> quantification across several established colorimetric assays. Our results reveal that quantification inaccuracies arise from a combination of factors, including pre-existing H<sub>2</sub>O<sub>2</sub> contamination, spectral overlap, unintended redox reactions, and self-sensitization effects. Drawing from these findings, we propose practical guidelines for selecting compatible sacrificial agents, detection methods, and excitation wavelengths to minimize analytical artifacts and enable accurate evaluation of photocatalytic H<sub>2</sub>O<sub>2</sub> production.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"47 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144533821","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":"Manipulating the Potential Diagram for Better Lithium–Metal Batteries","authors":"Zhong Fang, Seongjae Ko, Atsuo Yamada","doi":"10.1021/acsenergylett.5c00832","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00832","url":null,"abstract":"Achieving high reversibility in Li-metal batteries, promising candidates for high-energy-density storage systems, remains a major challenge. This study addresses this by optimizing a full-cell potential diagram based on electrolyte energetics. Variations in Coulomb interactions among Li<sup>+</sup>, anions, and solvents in the electrolyte can affect (1) the electrostatic potential (liquid Madelung potential) of Li<sup>+</sup>, which can shift both the anode and cathode reaction potentials by the same magnitude; and (2) the operating potential window of the electrolyte, which can cause kinetic hindrance via the formation of a passivation film on the electrode. Systematically balancing these factors based on quantitative experimental results can enhance the performance of the Li-metal battery while minimizing electrolyte degradation at the electrode surface. These insights into the fundamental role of electrolyte energetics in battery design are expected to contribute to the development of comprehensive frameworks for highly stable high-energy-density storage devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"36 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144533816","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}
Zhikun Liu, Han Shi, Chenqiang Song, Jing Cui, Jing Hou, Zhenpeng Hu, Peng Kang
{"title":"Engineering Ligand-Functionalized Layers for Enhanced Fe2+ Capture and Stable Deposition in All-Iron Flow Batteries","authors":"Zhikun Liu, Han Shi, Chenqiang Song, Jing Cui, Jing Hou, Zhenpeng Hu, Peng Kang","doi":"10.1021/acsenergylett.5c01049","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01049","url":null,"abstract":"All-iron aqueous redox flow battery (ARFB) is a promising candidate for next-generation large-scale energy storage, due to low cost and environmental benignity, but the low reversibility of the Fe anode limits its long-term cycling stability. Herein, a 3-mercaptopropionic acid (MPA) ligand-functionalized layer (LFL) is utilized to achieve a highly reversible Fe-MPA anode. The MPA LFL not only minimizes corrosion and hydrogen evolution in acidic electrolyte, but also actively captures Fe<sup>2+</sup> ions and controls interfacial deposition. Specifically, the MPA LFL homogenizes Fe<sup>2+</sup> ion flux at the electrode interface, acting as a regulator that suppresses the dendritic iron growth and facilitates the reversible anode plating/stripping. Consequently, the all-iron ARFB based on the Fe-MPA anode delivers high Coulombic efficiency of ∼99.5% and energy efficiency of ∼75% over 330 h at 20 mA cm<sup>–2</sup>. This study highlights the strategy of designing function-oriented ligand-electrode interface for improving the stability of ARFBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"27 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144521088","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}
Beining Dong, Yuhong Jiang, Xinwei Guan, Xiaoran Zheng, Songyan Yin, Bin Gong, Tao Wan, Tingting Mei, Fandi Chen, Zhi Li, Mengyao Li, Aoning Yang, Owais Ahmad, Wonseok Chae, Jonghoon Han, Chao Chen, Liang Gao, Jincheol Kim, Chun-Ho Lin, Gang Wang, Yuerui Lu, Shujuan Huang, Tom Wu, Dewei Chu, Long Hu
{"title":"Quantum Dot Enabled Cation Exchange in Halide Perovskites for Photovoltaics and Infrared Photodetectors","authors":"Beining Dong, Yuhong Jiang, Xinwei Guan, Xiaoran Zheng, Songyan Yin, Bin Gong, Tao Wan, Tingting Mei, Fandi Chen, Zhi Li, Mengyao Li, Aoning Yang, Owais Ahmad, Wonseok Chae, Jonghoon Han, Chao Chen, Liang Gao, Jincheol Kim, Chun-Ho Lin, Gang Wang, Yuerui Lu, Shujuan Huang, Tom Wu, Dewei Chu, Long Hu","doi":"10.1021/acsenergylett.5c01321","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01321","url":null,"abstract":"Tailoring the photophysical properties of halide perovskites is a promising strategy to simultaneously address defects, modulate carrier dynamics, and expand the spectral response. Quantum dots (QDs) are promising candidates to functionalize perovskites; however, the interaction mechanisms between robust-lattice QDs and ionic perovskites remain unclear. Here, we pioneer a cation exchange approach using CdSe QDs to functionalize lead halide perovskites, where Cd<sup>2+</sup> replaces Pb<sup>2+</sup> and diffuses throughout the perovskite matrix. This cation exchange achieves dual benefits: (1) efficient defect passivation via Cd<sup>2–</sup> diffusion and Se<sup>2–</sup> coordination with undercoordinated Pb<sup>2+</sup>, and (2) extended infrared light response up to 1200 nm attributed to <i>in situ</i> formed PbSe QDs. The champion perovskite solar cells delivered a power conversion efficiency of 24.8%, significantly outperforming the control devices (23.0%). Moreover, infrared PbSe QDs formed enable broadband detection to infrared spectrum (300–1200 nm), with a detectivity of 2.9 × 10<sup>11</sup> Jones at 1170 nm under −0.3 V bias. Extension of this strategy to CdS QDs further confirmed this cation exchange mechanism. Therefore, our work establishes a versatile, scalable interface-engineering method between robust-lattice QDs and perovskites, paving the way for multifunctional optoelectronic applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144520918","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}
Chen-Jui Huang, Jin An Sam Oh, Marta Vicencio, Tianchen Hu, Hedi Yang, James N. Burrow, Yen-Fang Song, Gung-Chian Yin, Pavel Shevchenko, Kamila M. Wiaderek, Bing Joe Hwang, Ying Shirley Meng
{"title":"X-ray Micro-Computed Tomography for Structural Analysis of All-Solid-State Battery at Pouch Cell Level","authors":"Chen-Jui Huang, Jin An Sam Oh, Marta Vicencio, Tianchen Hu, Hedi Yang, James N. Burrow, Yen-Fang Song, Gung-Chian Yin, Pavel Shevchenko, Kamila M. Wiaderek, Bing Joe Hwang, Ying Shirley Meng","doi":"10.1021/acsenergylett.5c00956","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00956","url":null,"abstract":"Characterizing the microstructure of all-solid-state batteries (ASSBs) during fabrication and operation is vital for their advancement, particularly as scaling to pouch cell levels introduces challenges in probing large-scale microstructural evolution. This work highlights the potential of synchrotron X-ray micro-computed tomography (sXCT) as a nondestructive, rapid (<30 min), and high-resolution technique for visualizing and quantifying key microstructural features, including overhang, porosity, contact loss, active surface area, and tortuosity, in all-solid-state pouch cells. The large field of view (up to millimeters) of sXCT enables detailed analysis at an industry-relevant scale, bridging the gap between laboratory research and commercial applications. Furthermore, integrating realistic sXCT-derived 3D models into multiphysics simulations could provide insights into chemo-mechanical degradation, particularly at the edges of the pouch cells, offering a pathway for designing robust, high-performance ASSBs. This perspective establishes sXCT as an indispensable tool for advancing both the understanding and the engineering of next-generation energy storage systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144520917","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}
Xiangyang Li, Yuyang Wang, Hui Wang, Chen Chen, Shuai Zeng, Hailin Guo, Lingfeng Dong, Wei Li, Dan Liu, Fabao Li, Tao Wang
{"title":"Indacenodithieno[3,2-b]thiophene-Bridged Fullerene for Defect Suppression in Perovskite Photovoltaics","authors":"Xiangyang Li, Yuyang Wang, Hui Wang, Chen Chen, Shuai Zeng, Hailin Guo, Lingfeng Dong, Wei Li, Dan Liu, Fabao Li, Tao Wang","doi":"10.1021/acsenergylett.5c01599","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01599","url":null,"abstract":"Defects at the bulk and grain boundaries of perovskites, along with weak n-type surface characteristics, remain critical obstacles to enhance the power conversion efficiency (PCE) of the perovskite solar cells (PSCs). Herein, an acceptor–donor–acceptor (A-D-A) type organic passivator structured with two C<sub>60</sub> cages sandwiching a nonfullerene acceptor fragment indacenodithieno[3,2-<i>b</i>]thiophene (IT), namely C<sub>60</sub>-IT-C<sub>60</sub>, is designed. Morphological and spectroscopic measurements demonstrate that the S element in the IT unit and the fullerene cages of C<sub>60</sub>-IT-C<sub>60</sub> act as a Lewis base and acid to passivate the uncoordinated Pb<sup>2+</sup> cation and anion defects. This interaction not only aligns the energy diagram and work functions of perovskite, but also encourages the crystallization of perovskite and suppresses the deep- and shallow-level defects, leading to a maximum PCE of 24.16% (fill factor of 84.75%) with improved storage and thermal stability in the corresponding PSCs. This work provides a new design paradigm of fullerene derivatives in PSCs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144520922","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}