{"title":"Realizing Surface Spin Configurations of Two-Dimensional Fe7S8 for Oxygen Evolution Reaction","authors":"Tingfeng Li, Wenda Zhou, Chao Zhong, Xingfang Luo, Ce Hu, Zhenzhen Jiang, Hang Zhou, Yong Yang, Ting Yu, Wen Lei, Cailei Yuan","doi":"10.1021/acsenergylett.5c00059","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00059","url":null,"abstract":"The surface spin configuration of catalysts is crucial for spin-dependent catalysis, as electrochemical reactions predominantly occur at the solid–liquid interface. This configuration influences reaction efficiency by altering the spin states of intermediates. Thus, identifying the surface spin configuration is essential for understanding the mechanisms affecting catalytic activity. This work designs multidomain and single-domain Fe<sub>7</sub>S<sub>8</sub> nanosheets through thickness control. Under a 200 mT magnetic field, the multidomain sample transitions to a single-domain state, while the surface spin configuration of the single-domain sample remains unchanged, as observed via magnetic force microscopy. Electrochemical tests show that a saturated magnetic field of 200 mT reduces the overpotential of the multidomain sample from 306 to 240 mV at 10 mA cm<sup>–2</sup>, while the single-domain sample maintains an overpotential of 257 mV. These results demonstrate that spin disorder at magnetic domain walls limits spin selectivity during the OER, suggesting strategies for developing innovative spin-selective catalysts.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"14 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143030883","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":"Scaling Direct Recycling of Lithium-Ion Batteries toward Industrialization: Challenges and Opportunities","authors":"Jiao Lin, Wei Li, Zheng Chen","doi":"10.1021/acsenergylett.4c03176","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03176","url":null,"abstract":"Lithium-ion batteries (LIBs) are indispensable for modern technology, yet their limited lifespan contributes substantially to electronic waste. Effective recycling methods are crucial to mitigating material scarcity, enhancing sustainability, and fostering a circular economy. This perspective examines the current LIB recycling processes, with a focus on the emerging potential and challenges of direct recycling methods. Unlike traditional pyrometallurgy and hydrometallurgy, which often destroy valuable materials, direct recycling seeks to recover and restore functional components, preserving the integrity of active materials. However, this method faces significant technical hurdles, particularly due to the complex design of LIBs and the degradation of key components over time. This perspective explores the intricacies of battery structure and component degradation, examines the challenges of scaling up direct recycling for industry applications, and proposes future directions to improve the efficiency and viability of this sustainable recycling approach.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"27 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143030960","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":"Quasi-Planar Heterojunction: Enhancing Stability and Practicality in Organic Photovoltaics","authors":"Yiwu Zhu, Feng He","doi":"10.1021/acsenergylett.4c03046","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03046","url":null,"abstract":"With the rapid advancements in the power conversion efficiency (PCE) of organic photovoltaic (OPV) devices, their stability has garnered increasing attention. While material innovation has played a critical role in recent years, the Q-PHJ (quasi-planar heterojunction) architecture offers an alternative approach to device optimization. This article aims to explain how the introduction of the Q-PHJ architecture can mitigate degradation under various conditions without compromising device performance. It begins by illustrating the fundamental mechanisms responsible for the degradation of OPV devices. Following this, the advantages of the Q-PHJ device and the mechanism are explained by introducing our recent work as well as highlighting other researchers’ work in this field. Different aspects and factors such as morphology, the ternary strategy, additive engineering, and vertical distribution were analyzed. The role of material innovation is also discussed. In the end, the feasibility and challenges of applying bilayer and bilayer-dominated devices to industrial manufacturing are analyzed in detail.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"38 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143026801","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}
Mengde Zhai, Kaihuai Du, Chengyang Liu, Cheng Chen, Guixiang Li, Haoxin Wang, Ziyang Xia, Jinman Yang, Hui Xu, Aili Wang, Toshinori Matsushima, Zhanglin Guo, Meng Li, Antonio Abate, Paul J. Dyson, Mohammad Khaja Nazeeruddin, Ming Cheng
{"title":"Fluorene-Terminated π-Conjugated Spiro-Type Hole Transport Materials for Perovskite Solar Cells","authors":"Mengde Zhai, Kaihuai Du, Chengyang Liu, Cheng Chen, Guixiang Li, Haoxin Wang, Ziyang Xia, Jinman Yang, Hui Xu, Aili Wang, Toshinori Matsushima, Zhanglin Guo, Meng Li, Antonio Abate, Paul J. Dyson, Mohammad Khaja Nazeeruddin, Ming Cheng","doi":"10.1021/acsenergylett.4c03233","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03233","url":null,"abstract":"Spiro-OMeTAD is a widely used hole transport material (HTM) in perovskite solar cells (PSCs), but its inherent low hole mobility and poor thermal stability affect the overall performance of PSCs. To overcome these limitations, we develop a series of fluorene-terminated Spiro-type HTMs, engineered by modulating the fluorene substitution site and π-conjugated intensity. Among these, the <i>p</i>-BM material exhibits high energetic ordering in film, appropriate energy levels, and efficient carrier extraction, enabling PSCs to achieve power conversion efficiencies (PCEs) of 25.5% and 24.03% for aperture areas of 0.0625 and 1 cm<sup>2</sup>, respectively. Additionally, a perovskite solar mini-module (size 16 cm<sup>2</sup>) based on <i>p</i>-BM HTM achieved a PCE of 22.4%. More importantly, <i>p</i>-BM exhibits a high glass transition temperature and enhanced film hydrophobicity, significantly improving the stability of devices in relation to heat and humidity. Our findings provide a promising alternative HTM for developing efficient and stable perovskite photovoltaic devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"39 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143019992","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}
Shixuan Liu, Di Wu, Minghua Kong, Wu Wang, Lin Xie, Jiaqing He
{"title":"High-Entropy Thermoelectric Materials: Advances, Challenges, and Future Opportunities","authors":"Shixuan Liu, Di Wu, Minghua Kong, Wu Wang, Lin Xie, Jiaqing He","doi":"10.1021/acsenergylett.4c03369","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03369","url":null,"abstract":"Thermoelectric conversion technology can realize direct conversion between heat and electricity, providing a promising approach to relieve the energy crisis. The application of thermoelectric technology is closely related to materials’ thermoelectric and mechanical properties. However, the strong coupling of key parameters involving charge carriers and phonon transport hinders the substantial improvements in overall thermoelectric performance. In recent years, a high-entropy strategy promoted remarkable progress in the field of thermoelectric materials by leveraging the four core effects. In this review, we first discuss the theoretical basis for how a high-entropy strategy synergistically optimizes thermoelectric performance. We then classify the examples where high-entropy effects can optimize electrical, thermal, and mechanical properties in thermoelectric materials. Following this, we summarize the overall advances that the high-entropy strategy has brought to thermoelectric materials and devices. Finally, we point out the remaining challenges in high-entropy thermoelectrics and offer perspectives on future research directions in this field.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"82 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143019994","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":"Rationalizing Light-Induced Phase Segregation Reversal by Halide Oxidation and Diffusion in Mixed Halide Perovskites","authors":"Nuerbiya Aihemaiti, Siying Peng","doi":"10.1021/acsenergylett.4c03073","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03073","url":null,"abstract":"Lead halide perovskites are one of the most promising materials as active layers of optoelectronic devices. Phase segregation under illumination in mixed halide perovskites is one of the major issues in stable device operation. Herein, we rationalize illumination power dependent phase segregation phenomena, including two thresholds between which phase segregation occurs, and the reversal of phase segregation. Our experimental observation combining confocal photoluminescence mapping with in situ Raman spectroscopy supports the halide oxidation model. We observed phase segregation beyond the illuminated area, while the illuminated area remained mixed. Reversal of phase segregation under illumination was also observed. We propose that the spatial distribution of phase segregation is driven by halide oxidation and diffusion of the products through mass flow, as verified by light- and spatial-dependent lattice halide vibrations. Our insights into phase segregation may provide new perspectives for manipulating phase segregation by local light intensity for dynamically tunable optoelectronics.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"28 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143019995","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":"Electrochemical Grain Refinement Enables High-Performance Lithium–Aluminum-Anode-Based All-Solid-State Batteries","authors":"Lun Zhang, Xuedong Zhang, Baiyu Guo, Zhaoyu Rong, Zhihao Yan, Bo Wang, Menglin Li, Zhenyu Wang, Lingyun Zhu, Qiao Huang, Yongfu Tang, Jianyu Huang","doi":"10.1021/acsenergylett.4c03250","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03250","url":null,"abstract":"Lithium–aluminum (Li<sub><i>x</i></sub>Al, <i>x</i> = the molar ratio of Li to Al), an important alloy anode with a specific capacity over 2 times higher than that of the carbon anode used in commercial liquid electrolyte lithium-ion batteries (LELIBs), has been proven to be a failure in LELIBs due to the notorious pulverization phenomenon. However, whether or not such pulverization persists in all solid state lithium batteries (ASSLBs) remains unclear. Herein, we show that pulverization of the Li<sub><i>x</i></sub>Al anode is mitigated in ASSLBs due to the applied external stack pressure, thus preventing the mechanical failure of the Li<sub><i>x</i></sub>Al anode in ASSLBs. Moreover, electron microscopy investigation reveals that, instead of pulverization, electrochemomechanical stress induces 2 orders of magnitude grain size reduction from a few tens of microns to a few hundred nanometers. The grain-refined Li<sub><i>x</i></sub>Al anode facilitates lithium ion transport, which improves the rate performance and specific capacity of the Li<sub><i>x</i></sub>Al anode. Consequently, the assembled single-crystal LiNi<sub>0.83</sub>Co<sub>0.12</sub>Mn<sub>0.05</sub>O<sub>2</sub>|Li<sub>10</sub>Si<sub>0.3</sub>PS<sub>6.7</sub>Cl<sub>1.8</sub>|Li<sub>0.4</sub>Al ASSLBs reach 2000 cycles with a capacity retention of 100% at 3C (13.9 mA/cm<sup>2</sup>, room temperature), at a high areal capacity of 2.1 mAh/cm<sup>2</sup>. The all-solid pouch cell with a Li<sub><i>x</i></sub>Al anode can reach an energy density of 219 Wh kg<sup>–1</sup> based on the total mass of the cell. These results demonstrate the prospect of implementing the Al-based anode in ASSLBs for practical energy storage applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"49 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143019996","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}
Haoran Zhou, Md Aftabuzzaman, Masud, Sung Ho Kang, Hwan Kyu Kim
{"title":"Key Materials and Fabrication Strategies for High-Performance Dye-Sensitized Solar Cells: Comprehensive Comparison and Perspective","authors":"Haoran Zhou, Md Aftabuzzaman, Masud, Sung Ho Kang, Hwan Kyu Kim","doi":"10.1021/acsenergylett.4c03579","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03579","url":null,"abstract":"For more than three decades, dye-sensitized solar cells (DSSCs) have attracted numerous researchers as viable alternatives in photovoltaic technology. It offers several advantages, such as using eco-friendly materials, inexpensive processing techniques, indoor photovoltaic potentials, and integrating photovoltaics into building applications. Nevertheless, DSSCs will require further development in manufacturing methods and materials to remain competitive with other thin-film solar technologies that offer high photovoltaic efficiency. It is essential to give an overview of the latest developments in this area and highlight the primary elements required for realizing high-performance technologies, such as photoanode modification, dye formulation, and electrolyte optimization. Recent advancements have shown promising improvements in DSSCs with copper-based electrolytes, and integrating new interface materials like preadsorbents or postadsorbents has also opened new possibilities for DSSCs. Here, we comprehensively compare and discuss the key materials and device fabrication processes for high-performance DSSCs and present future research perspectives.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"50 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143019998","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}
Yunya Zhang, Wurigumula Bao, Ethan Jeffs, Bin Liu, Bing Han, Weijie Mai, Xinyu Li, Weikang Li, Yun Xu, Bhargav Bhamwala, Alex Liu, Louis Ah, Kun Ryu, Ying Shirley Meng, Hong Gan
{"title":"Unveiling the Impacts of Charge/Discharge Rate on the Cycling Performance of Li-Metal Batteries","authors":"Yunya Zhang, Wurigumula Bao, Ethan Jeffs, Bin Liu, Bing Han, Weijie Mai, Xinyu Li, Weikang Li, Yun Xu, Bhargav Bhamwala, Alex Liu, Louis Ah, Kun Ryu, Ying Shirley Meng, Hong Gan","doi":"10.1021/acsenergylett.4c03215","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03215","url":null,"abstract":"Lithium metal batteries (LMBs) offer superior energy density and power capability but face challenges in cycle stability and safety. This study introduces a strategic approach to improving LMB cycle stability by optimizing charge/discharge rates. Our results show that slow charging (0.2C) and fast discharging (3C) significantly improve performance, with a multilayer LMB retaining over 80% capacity after 1000 cycles. Fast discharge rates promote lithium plating beneath the SEI layer, suppressing its growth and improving Coulombic efficiency, whereas slow discharge rates facilitate lithium plating above the SEI, leading to SEI accumulation. We propose a rational hypothesis linking SEI conductivity and cycling conditions and introduce an intermittent pulse discharge protocol to emulate electric vehicle applications, further improving the stability. These optimized cycling strategies enhance the LMB lifespan, utility, and safety, paving the way for broader market adoption in the years ahead.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"33 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142992560","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":"Unlocking Ultrafast Diagnosis of Retired Batteries via Interpretable Machine Learning and Optical Fiber Sensors","authors":"Taolue Zhang, Ruifeng Tan, Pinxi Zhu, Tong-Yi Zhang, Jiaqiang Huang","doi":"10.1021/acsenergylett.4c03054","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03054","url":null,"abstract":"Retired batteries are of great economic and environmental importance, which are indispensable considerations in the life cycle of lithium-ion batteries. However, existing methods for evaluating retired batteries are time- and resource-consuming, hindering efficient screening for later recycling or reuse. Herein, combining optical fiber sensors and interpretable machine learning (ML), we establish a data-driven framework for retired battery datasets with 265 cells of different chemistries (LiFePO<sub>4</sub>/graphite, LiMn<sub>2</sub>O<sub>4</sub>/graphite) and achieve ultrafast state of health diagnosis within 3 min, offering mean absolute errors of 1.17% and 2.78%, respectively. The proposed data-driven framework identifies the salient regions in the time-resolved multivariable data and helps to uncover underlying thermodynamic/kinetic aging mechanisms. We also demonstrate the incorporated thermal information obtained via optical fibers complements voltage signals by improving prediction accuracy and antinoise ability. This work not only showcases the potential of battery sensing in retired battery diagnosis but also unlocks the unexplored synergy between sensing and interpretable ML for diverse battery applications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"71 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142990757","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}