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Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage 利用催化剂:支持酰胺键,从电ph位移的DAC捕获后液体中电合成CO
IF 38.6 1区 材料科学
Joule Pub Date : 2025-05-21 DOI: 10.1016/j.joule.2025.101883
Bei Zhou , Hengzhou Liu , Guangcan Su , Heejong Shin , Xiao-Yan Li , Huajie Ze , Yongxiang Liang , Bosi Peng , Weiyan Ni , Yuanjun Chen , Wenjin Zhu , Christine Yu , Yiqing Chen , Pengfei Ou , Ke Xie , Edward H. Sargent
{"title":"Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage","authors":"Bei Zhou ,&nbsp;Hengzhou Liu ,&nbsp;Guangcan Su ,&nbsp;Heejong Shin ,&nbsp;Xiao-Yan Li ,&nbsp;Huajie Ze ,&nbsp;Yongxiang Liang ,&nbsp;Bosi Peng ,&nbsp;Weiyan Ni ,&nbsp;Yuanjun Chen ,&nbsp;Wenjin Zhu ,&nbsp;Christine Yu ,&nbsp;Yiqing Chen ,&nbsp;Pengfei Ou ,&nbsp;Ke Xie ,&nbsp;Edward H. Sargent","doi":"10.1016/j.joule.2025.101883","DOIUrl":"10.1016/j.joule.2025.101883","url":null,"abstract":"<div><div>Electrified reactive capture upgrades CO<sub>2</sub> from post-air-capture alkali carbonate liquid to value-added products while regenerating the capture medium. Previous processes exhibited limited energy efficiency (&lt;18%) due to high full-cell voltage (&gt;3.7 V) and modest CO selectivity (&lt;45%). To address this, we developed a Co molecular catalyst featuring an electron-deficient Co center, lowering the required reduction voltage. We then grafted the catalyst onto a conductive support, enhancing charge transfer. An electrified pH-downshifter improved CO<sub>2</sub> availability, increasing CO selectivity. The system achieved 70% CO selectivity at 2.7 V and 100 mA cm<sup>−2</sup>, corresponding to an energy intensity of 35 GJ/ton CO. The energy cost is comparable to that of direct air capture (DAC) followed by reverse water-gas shift (RWGS), but it offers ambient temperature operation.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 5","pages":"Article 101883"},"PeriodicalIF":38.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703354","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}
引用次数: 0
Carbon contracts for difference design: Managing carbon price risk in a low-carbon industry 基于差异设计的碳合约:低碳产业的碳价格风险管理
IF 38.6 1区 材料科学
Joule Pub Date : 2025-05-21 DOI: 10.1016/j.joule.2025.101921
Alexander Hoogsteyn , Kenneth Bruninx , Erik Delarue
{"title":"Carbon contracts for difference design: Managing carbon price risk in a low-carbon industry","authors":"Alexander Hoogsteyn ,&nbsp;Kenneth Bruninx ,&nbsp;Erik Delarue","doi":"10.1016/j.joule.2025.101921","DOIUrl":"10.1016/j.joule.2025.101921","url":null,"abstract":"<div><div>Alexander Hoogsteyn obtained his MSc from KU Leuven in 2021 with a major in electrical engineering and minor in power system engineering. He then completed a traineeship at the EU Agency for Cooperation of Energy Regulators, after which he returned to KU Leuven to pursue a PhD in mechanical engineering at the Energy Systems Integration and Modeling research group. He is also affiliated with Energyville in Genk. Here, he investigates the role of hydrogen in industrial decarbonization and the impact hydrogen policies have on energy markets.</div><div>Kenneth Bruninx received MSc and PhD degrees in energy engineering in 2011 and 2016, respectively, and an MSc degree in management in 2015 from KU Leuven, Belgium. Currently, he is an associate professor at the Delft University of Technology (TU Delft) and a research fellow at KU Leuven. His main research interests include market design, policy, and regulation for integrated net-zero energy systems. He serves as the chair of the IEEE EPPC WG on Energy and is an associate editor of the <em>IEEE Transactions on Energy Markets, Policy &amp; Regulation</em>.</div><div>Erik Delarue received MSc and PhD degrees in mechanical engineering from KU Leuven, Belgium, in 2005 and 2009, respectively. He is a professor at KU Leuven, TME Branch (energy conversion), leading the Energy Systems Integration and Modeling research group, and he is active within EnergyVille. His research focus and expertise are on quantitative tools supporting an efficient operation of, and transition toward, a low-carbon energy system (mathematical modeling of energy systems). Applications relate to flexibility through energy systems integration, energy market design, and energy policies. Erik has published widely in the academic literature.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 5","pages":"Article 101921"},"PeriodicalIF":38.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143837045","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}
引用次数: 0
Sodium-mediated redox cascade for electrochemical ammonia synthesis 钠介导的氧化还原级联电化学合成氨
IF 38.6 1区 材料科学
Joule Pub Date : 2025-05-21 DOI: 10.1016/j.joule.2025.101923
Channing K. Klein , Alexis Lindenfelser , Michael A. Yusov , Anukta Jain , Ryan J.R. Jones , John Gregoire , Karthish Manthiram
{"title":"Sodium-mediated redox cascade for electrochemical ammonia synthesis","authors":"Channing K. Klein ,&nbsp;Alexis Lindenfelser ,&nbsp;Michael A. Yusov ,&nbsp;Anukta Jain ,&nbsp;Ryan J.R. Jones ,&nbsp;John Gregoire ,&nbsp;Karthish Manthiram","doi":"10.1016/j.joule.2025.101923","DOIUrl":"10.1016/j.joule.2025.101923","url":null,"abstract":"<div><div>Artificial ammonia synthesis is vital to modern life; however, the Haber-Bosch process, by which most ammonia is synthesized, is capital and carbon intensive. Zero-valent-metal-mediated ammonia synthesis is a promising alternative but requires a metal that is both a strong reductant and forms a stable nitride. Only a small number of metals, like lithium, can satisfy these constraints. Therefore, we developed an electrochemical paradigm enabling the use of different reductants by orthogonalizing the roles of the zero-valent metal between sodium metal and a Ti active site. These components are cheaper than lithium by two orders of magnitude. Using a sodium-naphthalene-titanium cascade, we achieved a rate of 475 nmol cm<sup>−2</sup> s<sup>−1</sup> and a Faradaic efficiency of 24% and found that the reaction rate depends primarily on current density.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 5","pages":"Article 101923"},"PeriodicalIF":38.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858173","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}
引用次数: 0
Neighboring nonmetal site as an intermediate modulator switching CO2 electroreduction pathway toward multicarbons 邻近非金属位作为中间调制器,将CO2电还原途径转换为多碳
IF 38.6 1区 材料科学
Joule Pub Date : 2025-05-21 DOI: 10.1016/j.joule.2025.101926
Li Li , Ying Zhou , Chaofan Wan , Xiaodong Li , Panzhe Qiao , Shibo Xi , Yan Fang , Xianbiao Fu , Jiexin Zhu , Shumin Wang , Xia Wang , Chengbin Xu , Zechao Zhuang , Ming Zuo , Minghui Fan , Zheng Jiang , Wenhua Zhang , Xinliang Feng , Yongfu Sun , Jinlong Yang , Yi Xie
{"title":"Neighboring nonmetal site as an intermediate modulator switching CO2 electroreduction pathway toward multicarbons","authors":"Li Li ,&nbsp;Ying Zhou ,&nbsp;Chaofan Wan ,&nbsp;Xiaodong Li ,&nbsp;Panzhe Qiao ,&nbsp;Shibo Xi ,&nbsp;Yan Fang ,&nbsp;Xianbiao Fu ,&nbsp;Jiexin Zhu ,&nbsp;Shumin Wang ,&nbsp;Xia Wang ,&nbsp;Chengbin Xu ,&nbsp;Zechao Zhuang ,&nbsp;Ming Zuo ,&nbsp;Minghui Fan ,&nbsp;Zheng Jiang ,&nbsp;Wenhua Zhang ,&nbsp;Xinliang Feng ,&nbsp;Yongfu Sun ,&nbsp;Jinlong Yang ,&nbsp;Yi Xie","doi":"10.1016/j.joule.2025.101926","DOIUrl":"10.1016/j.joule.2025.101926","url":null,"abstract":"<div><div>Selective CO<sub>2</sub> electroreduction toward multicarbons (C<sub>2+</sub>) is hampered by the competing pathways at ampere-level current densities. Here, theoretical calculations reveal that the binding strength and protonation of the ∗CO intermediate are a pair of key descriptors in governing the selectivity-determining bifurcation pathway on copper (Cu) catalyst. Hence, we propose an intermediate-modulator strategy with a nonmetallic phosphorus (P)-modified Cu (P-Cu) hetero-site catalyst for ideal C<sub>2+</sub> formation. The P site enhances charge accumulation at the neighboring Cu site, which strengthens ∗CO adsorption and active ∗H supply from H<sub>2</sub>O activation, favoring a rich-∗H-assisted-protonation (RHP) pathway toward ∗CHO formation. Subsequently, the lowest-energy-barrier ∗CO-∗CHO coupling pathway switches the predominant reaction pathway away from undesired CO and H<sub>2</sub> to higher-value ethylene and ethanol. We report a C<sub>2+</sub> partial current density of 1.05 A cm<sup>−2</sup> and a Faradaic efficiency of 87.7%. Utilizing cheaper nonmetallic elements, this catalyst design principle outperforms reported outcomes with precious metal dopants.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 5","pages":"Article 101926"},"PeriodicalIF":38.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862362","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}
引用次数: 0
Is oxidation of dinitrogen at measurable rates possible under mild conditions? 在温和的条件下,二氮是否有可能以可测量的速率氧化?
IF 38.6 1区 材料科学
Joule Pub Date : 2025-05-21 DOI: 10.1016/j.joule.2025.101924
Mattia Belotti , Felipe Matamala-Troncoso , Alasdair I. McKay , Thi Mung Vu , Douglas R. MacFarlane , Alexandr N. Simonov
{"title":"Is oxidation of dinitrogen at measurable rates possible under mild conditions?","authors":"Mattia Belotti ,&nbsp;Felipe Matamala-Troncoso ,&nbsp;Alasdair I. McKay ,&nbsp;Thi Mung Vu ,&nbsp;Douglas R. MacFarlane ,&nbsp;Alexandr N. Simonov","doi":"10.1016/j.joule.2025.101924","DOIUrl":"10.1016/j.joule.2025.101924","url":null,"abstract":"<div><div>Chemical activation of dinitrogen (N<sub>2</sub>) gas is well established via reductive pathways in catalytic, electrochemical, and biochemical modes. In contrast, the possibility of N<sub>2</sub> oxidation has only been unambiguously proven under extreme conditions, such as those provided by lightning or plasma discharge. Nevertheless, attempts to oxidize N<sub>2</sub> under mild conditions using electro- and photo-catalysis are being undertaken and regularly reported to produce putatively positive outcomes. The present article aims to (1) critically assess the actual status of the field of N<sub>2</sub> oxidation under close-to-ambient conditions, (2) propose an experimental methodology that substantially decreases the probability of false-positive results, and (3) explore some of the apparently promising approaches to N<sub>2</sub> oxidation at temperatures below 100°C. We conclude that no experiments reported so far, including ours, were able to unambiguously prove the possibility of N<sub>2</sub> oxidation under mild conditions.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 5","pages":"Article 101924"},"PeriodicalIF":38.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143880886","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}
引用次数: 0
Marshalling our productivity to create a sustainable global civilization 整合我们的生产力,创造一个可持续的全球文明
IF 38.6 1区 材料科学
Joule Pub Date : 2025-05-21 DOI: 10.1016/j.joule.2025.101929
Ian Marius Peters , Christian Breyer
{"title":"Marshalling our productivity to create a sustainable global civilization","authors":"Ian Marius Peters ,&nbsp;Christian Breyer","doi":"10.1016/j.joule.2025.101929","DOIUrl":"10.1016/j.joule.2025.101929","url":null,"abstract":"<div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (76KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span>Ian Marius Peters is a physicist with over 20 years of experience in photovoltaic research. He has authored more than 300 scientific publications on sustainable energy systems, photovoltaic (PV) technologies, artificial intelligence in energy, and solar cost modeling. His career spans leading institutions including Fraunhofer ISE, SERIS, and MIT. He currently heads the High Throughput Field Inspections and Recycling group at the Helmholtz Institute Erlangen-Nuremberg for Renewable Energy (HI-ERN), part of Forschungszentrum Jülich. Dr. Peters received the 2021 Hamakawa Award for his contributions to PV energy conversion and a 2023 ERC Consolidator Grant for PV cradle-to-cradle recycling research.</div><div><span><figure><span><img><ol><li><span><span>Download: <span>Download high-res image (95KB)</span></span></span></li><li><span><span>Download: <span>Download full-size image</span></span></span></li></ol></span></figure></span>Christian Breyer is professor of solar economy at LUT University, Finland, specializing in high-resolution modeling of 100% renewable energy systems across all sectors and scales. He has published over 400 scientific papers, including more than 200 journal articles, with research focused on integrated power, heat, transport, industry, and power-to-X solutions. His team leads globally in studies on fully renewable energy transitions. Previously, he worked at Reiner Lemoine Institut and Q-Cells. He serves on numerous scientific and policy advisory boards, including ETIP PV, IEA-PVPS, and the IPCC. Prof. Breyer holds a PhD in electrical engineering and has a multidisciplinary academic background.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 5","pages":"Article 101929"},"PeriodicalIF":38.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143893519","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}
引用次数: 0
Susceptible organic cations enable stable and efficient perovskite solar cells 易感有机阳离子使钙钛矿太阳能电池稳定高效
IF 38.6 1区 材料科学
Joule Pub Date : 2025-05-21 DOI: 10.1016/j.joule.2025.101879
Jongbeom Kim , Jaewang Park , Jihoo Lim , Jaehui Kim , Junseok Kim , Nahye Shin , Jae Sung Yun , Jino Im , Sang Il Seok
{"title":"Susceptible organic cations enable stable and efficient perovskite solar cells","authors":"Jongbeom Kim ,&nbsp;Jaewang Park ,&nbsp;Jihoo Lim ,&nbsp;Jaehui Kim ,&nbsp;Junseok Kim ,&nbsp;Nahye Shin ,&nbsp;Jae Sung Yun ,&nbsp;Jino Im ,&nbsp;Sang Il Seok","doi":"10.1016/j.joule.2025.101879","DOIUrl":"10.1016/j.joule.2025.101879","url":null,"abstract":"<div><div>Achieving higher open-circuit voltages and fill factors in perovskite solar cells (PSCs) involves minimizing defects between layers and maximizing carrier extraction and transport. One approach includes integrating a two-dimensional (2D) semiconducting interlayer to form a heterojunction with the perovskite absorber. However, conventional 2D layers often have poor thermal stability due to the migration of organic cations. This study examines the enhancement in power conversion efficiency (PCE) and thermal stability of PSCs by using strong intermolecular interactions between methoxy-phenethylammonium iodide and cyclohexylammonium bromide as chosen organic cations. The resulting 2D/perovskite configuration facilitates efficient charge transfer and demonstrates superior thermal stability at 85°C. The optimized PSCs achieved a PCE of 26.28% under air mass (AM) 1.5G illumination, retaining 88% efficiency after 440 h of continuous illumination and maintaining 100% of its initial efficiency after 9,000 h under ambient conditions. This research contributes to developing highly efficient and stable PSCs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 5","pages":"Article 101879"},"PeriodicalIF":38.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635646","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}
引用次数: 0
Dynamic evolution of cathode-electrolyte interphase in lithium metal batteries with ether electrolytes 含醚电解质的锂金属电池阴极-电解质界面的动态演化
IF 38.6 1区 材料科学
Joule Pub Date : 2025-05-21 DOI: 10.1016/j.joule.2025.101885
Yawei Chen , Menghao Li , Yulin Jie , Yue Liu , Zhengfeng Zhang , Peiping Yu , Wanxia Li , Yang Liu , Xinpeng Li , Zhanwu Lei , Pengfei Yan , Tao Cheng , M. Danny Gu , Shuhong Jiao , Ruiguo Cao
{"title":"Dynamic evolution of cathode-electrolyte interphase in lithium metal batteries with ether electrolytes","authors":"Yawei Chen ,&nbsp;Menghao Li ,&nbsp;Yulin Jie ,&nbsp;Yue Liu ,&nbsp;Zhengfeng Zhang ,&nbsp;Peiping Yu ,&nbsp;Wanxia Li ,&nbsp;Yang Liu ,&nbsp;Xinpeng Li ,&nbsp;Zhanwu Lei ,&nbsp;Pengfei Yan ,&nbsp;Tao Cheng ,&nbsp;M. Danny Gu ,&nbsp;Shuhong Jiao ,&nbsp;Ruiguo Cao","doi":"10.1016/j.joule.2025.101885","DOIUrl":"10.1016/j.joule.2025.101885","url":null,"abstract":"<div><div>High-voltage lithium (Li) metal batteries (HVLMBs) have attracted tremendous research interest in the past decade owing to their high energy densities. Electrode-electrolyte interphases in HVLMBs play critical roles in dictating their electrochemical performance. However, despite the intensive research on solid-electrolyte interphase (SEI) of Li anode, the cathode-electrolyte interphase (CEI) on high-voltage cathodes remains elusive. Herein, we report the formation and dynamic evolution of CEI on LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) cathodes in ether-based electrolytes. We reveal that the solvent-derived interphase predominates the initial CEI, which subsequently evolves into a Li fluoride (LiF)-rich CEI during cycling. Through solvent design, the weak-solvation electrolyte with branched ether solvents promotes the formation of a conformal CEI layer featuring the monodispersing LiF nanocrystals (∼8 nm), thereby enabling NMC811 cathodes to sustain up to 2,000 cycles. This work addresses the long-standing questions regarding CEI evolution and provides valuable guidance for the rational electrolyte design for HVLMBs.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 5","pages":"Article 101885"},"PeriodicalIF":38.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713656","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}
引用次数: 0
Efficient and stable high-entropy organic photovoltaics 高效稳定的高熵有机光伏
IF 38.6 1区 材料科学
Joule Pub Date : 2025-04-16 DOI: 10.1016/j.joule.2025.101851
Ming Zhang (张明) , Lei Zhu , Jun Yan , Xiaonan Xue , Zaiyu Wang , Flurin Eisner , Guanqing Zhou , Rui Zeng , Lixuan Kan , Liang Wu , Wenkai Zhong , Anyang Zhang , Fei Han , Jingnan Song , Nicolai Hartmann , Zichun Zhou , Hao Jing , Haiming Zhu , Shengjie Xu (许胜杰) , Jenny Nelson , Feng Liu (刘烽)
{"title":"Efficient and stable high-entropy organic photovoltaics","authors":"Ming Zhang (张明) ,&nbsp;Lei Zhu ,&nbsp;Jun Yan ,&nbsp;Xiaonan Xue ,&nbsp;Zaiyu Wang ,&nbsp;Flurin Eisner ,&nbsp;Guanqing Zhou ,&nbsp;Rui Zeng ,&nbsp;Lixuan Kan ,&nbsp;Liang Wu ,&nbsp;Wenkai Zhong ,&nbsp;Anyang Zhang ,&nbsp;Fei Han ,&nbsp;Jingnan Song ,&nbsp;Nicolai Hartmann ,&nbsp;Zichun Zhou ,&nbsp;Hao Jing ,&nbsp;Haiming Zhu ,&nbsp;Shengjie Xu (许胜杰) ,&nbsp;Jenny Nelson ,&nbsp;Feng Liu (刘烽)","doi":"10.1016/j.joule.2025.101851","DOIUrl":"10.1016/j.joule.2025.101851","url":null,"abstract":"<div><div>The lack of simultaneous high efficiency and long-term stability in organic photovoltaics (OPVs) poses a major challenge to commercialization. Here, we introduce a high-entropy (HE) methodology by both physical blending and chemical synthesis, where multiple components are mixed to improve system entropy. Our findings show that physically blended HE blends maintained strong π–π interactions due to acceptors’ identical backbones. The different halogens or alkyl chains reduced structure order and fostered an optimal mixture, where a redistribution of the conduction-band density of states was found, leading to a higher effective band gap, reduced non-radiative recombination, and elevated open-circuit voltage. This HE design rule was then extended to chemical synthesis to make HE materials, which yielded a maximum power conversion efficiency of 20.6% (20.3% ± 0.2%, certified as 20.0%) in OPV devices. Moreover, both operational and thermal stability were improved, measured in conventional encapsulated devices under continuous illumination.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101851"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539141","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}
引用次数: 0
Correlating electrode nano-confinement to interphase chemistry 电极纳米约束与相间化学的关系
IF 38.6 1区 材料科学
Joule Pub Date : 2025-04-16 DOI: 10.1016/j.joule.2025.101874
Guanjie Li , Dengpan Dong , Dmitry Bedrov , Qinqin Cai , Haojun Wu , Zixing Wang , Jilei Liu , Kang Xu , Lidan Xing , Weishan Li
{"title":"Correlating electrode nano-confinement to interphase chemistry","authors":"Guanjie Li ,&nbsp;Dengpan Dong ,&nbsp;Dmitry Bedrov ,&nbsp;Qinqin Cai ,&nbsp;Haojun Wu ,&nbsp;Zixing Wang ,&nbsp;Jilei Liu ,&nbsp;Kang Xu ,&nbsp;Lidan Xing ,&nbsp;Weishan Li","doi":"10.1016/j.joule.2025.101874","DOIUrl":"10.1016/j.joule.2025.101874","url":null,"abstract":"<div><div>The electrode/electrolyte interphases in advanced batteries are critical for their performance, influencing the reversibility and rate capability of cell reactions. Although much research has focused on the electrolyte side, our study reveals the significant impact of the electrode’s interlayer distance on interphasial chemistry. We discovered that smaller interlayer distances in graphitic anodes lead to higher sensitivity to co-intercalation of Li<sup>+</sup> and solvents, resulting in LiF-poor interphases that reduce stability. Conversely, larger interlayer distances allow anion-rich solvation structures, resulting in LiF-rich interphases and facilitating reversible intercalation/deintercalation reactions. This correlation between interlayer distance and interphasial chemistry offers new strategies for designing next-generation battery electrolytes and electrodes, moving beyond electrolyte engineering to include electrode structural considerations. Our findings are universally applicable across diverse electrolyte systems, providing a robust framework for optimizing battery performance.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101874"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618887","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}
引用次数: 0
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