ACS Energy Letters 最新文献_第4页

Eutectic Perturbations Enhance Multivalent-Cation Structural Diffusion in Salt-Concentrated Polymer Electrolytes

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-19 DOI: 10.1021/acsenergylett.4c02506

Guoli Lu, Jiaping Niu, Xiaofan Du, Chenyang Liu, Min Xing, Dongliang Chao, Yongping He, Lichun Ma, Zhihong Liu, Jingwen Zhao, Yaojian Zhang, Guanglei Cui

{"title":"Eutectic Perturbations Enhance Multivalent-Cation Structural Diffusion in Salt-Concentrated Polymer Electrolytes","authors":"Guoli Lu, Jiaping Niu, Xiaofan Du, Chenyang Liu, Min Xing, Dongliang Chao, Yongping He, Lichun Ma, Zhihong Liu, Jingwen Zhao, Yaojian Zhang, Guanglei Cui","doi":"10.1021/acsenergylett.4c02506","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02506","url":null,"abstract":"Cation transport in polymer electrolytes (PEs) is largely limited by insufficient segmental motion. Structural diffusion, often observed in salt-concentrated PEs, is emerging as an appealing transport mode for decoupling the correlation between ionic conductivity and polymer dynamics. However, due to inherently strong ionic association, realizing such a promise for multivalent cations remains challenging. We herein report a eutectic strategy that enhances the structural diffusion dynamics of divalent cations (e.g., Zn2+) in salt-concentrated polycationic PEs to approach levels comparable to those of monovalent cations. The strategic introduction of bipolar ligands (solid acetamide), eutectically inserting into the Zn2+-anion aggregates without directly plasticizing the polymeric skeleton, gives rise to local coordination distortions that weaken anionic traps on Zn2+ mobility. This eutectic perturbation further promotes microphase separation, creating expanded Zn2+ long-range percolating pathways independent of polymer backbones, enabling 3 orders of magnitude increase in ionic conductivity (to 2.4 × 10–5 S cm–1 at 30 °C) and supporting stable zinc metal cell cycling. Our strategy provides an alternative route toward molecular-scale controls over solid-phase conduction of charge-dense cations in PEs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"25 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858078","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

In Operando Visualization of Polymerized Ionic Liquid Electrolyte Migration in Solid-State Lithium Batteries

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-19 DOI: 10.1021/acsenergylett.4c02430

Bowen Chen, Ke Xu, Lingfei Tang, Qiang Li, Qi Chen, Liwei Chen

{"title":"In Operando Visualization of Polymerized Ionic Liquid Electrolyte Migration in Solid-State Lithium Batteries","authors":"Bowen Chen, Ke Xu, Lingfei Tang, Qiang Li, Qi Chen, Liwei Chen","doi":"10.1021/acsenergylett.4c02430","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02430","url":null,"abstract":"Polymerized ionic liquid (PIL) electrolytes with high flaming resistance, wide electrochemical stability window, and high flexibility have been widely explored for high safety, high energy density, and long-cycle lithium metal batteries (LMBs). Great efforts have been made in inhibiting anion movement in the PIL to increase the lithium transference number (tLi+), which reduces polarization loss and improves rate performance. However, the effect of tLi+ on the cycle performance is often overlooked because of self-limiting parasitic interfacial reactions involving anions. Here, PIL migration induced by mobile anions was visualized in operando via cross-sectional atomic force microscopy. Intense migration of the PIL with a low tLi+ breaks the interphase on electrodes and exacerbates anion decomposition, resulting in escalating interfacial impedance. The increased tLi+ inhibits interfacial electromechanical degradation and enhances cycle performance. This work reveals the pivotal but often unnoticed role of interfacial electro-mechanical coupling in PIL-based LMBs by taking advantages of in operando scrutiny of the buried interface.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"14 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858033","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

Tailoring C3N4 Host to Enable a High-Loading Iodine Electrode for High Energy and Long Cycling Zn–Iodine Battery

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-19 DOI: 10.1021/acsenergylett.4c02930

Wenwen Cao, Tao Hu, Yuanyuan Zhao, Zhenglin Li, Yichan Hu, Cuncheng Li, Yiqiang Sun, Feng Ding, Guojin Liang

{"title":"Tailoring C3N4 Host to Enable a High-Loading Iodine Electrode for High Energy and Long Cycling Zn–Iodine Battery","authors":"Wenwen Cao, Tao Hu, Yuanyuan Zhao, Zhenglin Li, Yichan Hu, Cuncheng Li, Yiqiang Sun, Feng Ding, Guojin Liang","doi":"10.1021/acsenergylett.4c02930","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02930","url":null,"abstract":"The high-energy-density zinc–iodine batteries (ZIBs) are hindered by low iodine loading in the cathode, which limited the specific capacity and energy density at the total electrode level. The unstable adsorption by the conventional host materials of the iodine electrode exacerbates the severe iodine shuttling and sluggish reaction kinetics. Here, we developed Br-doped carbon nitride (BrCN) nanosheets by using a chemical exfoliation strategy and doping engineering to obtain efficient iodine host materials for the iodine electrode. It eventually enhanced the adsorption force between BrCN and the iodine species, effectively stabilizing the high-loading iodine electrode and suppressing the polyiodide shuttle. As a result, BrCN-based host achieves an iodine mass loading of 14.1 mg cm–2 of 46 wt % mass loading ratio (up to a maximum loading of 23.5 mg cm–2), which achieves a high specific capacity of 97.0 mAh g–1 and the energy density of 116.4 Wh kg–1 based on the total iodine electrode.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"75 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858151","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

Suppressing Ionic-to-Electronic Conduction Transition on Cathode Interface Enables 4.4 V Poly(ethylene oxide)-Based All-Solid-State Batteries

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-18 DOI: 10.1021/acsenergylett.4c02840

Zi-Xiang Kong, Zhe Xiong, Jian-Fang Wu, Jun Jin, Yuxiao Lin, Yunsong Li, Jilei Liu

{"title":"Suppressing Ionic-to-Electronic Conduction Transition on Cathode Interface Enables 4.4 V Poly(ethylene oxide)-Based All-Solid-State Batteries","authors":"Zi-Xiang Kong, Zhe Xiong, Jian-Fang Wu, Jun Jin, Yuxiao Lin, Yunsong Li, Jilei Liu","doi":"10.1021/acsenergylett.4c02840","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02840","url":null,"abstract":"The implementation of energy-dense poly(ethylene oxide) (PEO)-based all-solid-state lithium batteries is impeded by the limited working voltage and underexplored cathode interfacial reaction mechanism. Here, through analyzing interfacial resistances using the Wagner model, the change of the interfacial reaction parameter (k) is proposed to unveil the ionic-to-electronic conduction transition and kinetic formation mechanism of the cathode-electrolyte-interphase (CEI) under voltage ≥4.2 V, thereby constructing ionic conductor-dominated CEIs to enable 4.4 V batteries. With the open-circuit voltage ≥4.2 V, k1 and k2 are derived; k2 is smaller than k1, caused by the enhanced electronic conduction and indicating the ionic-to-electronic conduction transition of the CEI. Moreover, by introducing LiPO2F2 in high-concentration solid electrolytes, ionic conductors Li3PO4 and LixPOFy dominate the CEI, overcoming the ionic-to-electronic conduction transition; the resulting 4.4 V cell bears a discharge capacity of 130 mAh/g with a retention of 90% after 100 cycles, about 2 times that of the normal PEO-based cell.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"63 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849655","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

Insights into Bubble Dynamics in Water Splitting 洞察水分离过程中的气泡动力学

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-17 DOI: 10.1021/acsenergylett.4c02736

Jaemin Park, Min Jae Kim, Youngeun Kim, Siyoung Lee, Sunghak Park, Wooseok Yang

引用次数: 0

A Practical Efficiency Target for Perovskite/Silicon Tandem Solar Cells

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-17 DOI: 10.1021/acsenergylett.4c02152

Thomas G. Allen, Esma Ugur, Erkan Aydin, Anand S. Subbiah, Stefaan De Wolf

引用次数: 0

Solvation Structure Engineering of Weakly Coordinating Sulfonamide Electrolytes for 4.6 V Lithium Metal Batteries 用于 4.6 V 金属锂电池的弱配位磺酰胺电解质的溶解结构工程设计

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-17 DOI: 10.1021/acsenergylett.4c03030

Lea Pompizii, Mingliang Liu, Leonie Braks, Timur Ashirov, Tianhong Zhou, Mounir Mensi, Dongmin Park, Jang Wook Choi, Ali Coskun

引用次数: 0

The Effect of Antisolvent Treatment on the Growth of 2D/3D Tin Perovskite Films for Solar Cells 反溶剂处理对用于太阳能电池的 2D/3D 锡过氧化物薄膜生长的影响

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-17 DOI: 10.1021/acsenergylett.4c02745

Ganghong Min, Robert J. E. Westbrook, Meihuizi Jiang, Margherita Taddei, Ang Li, Thomas Webb, Sanjayan Sathasivam, Amanz Azaden, Robert G. Palgrave, David S. Ginger, Thomas J. Macdonald, Saif A. Haque

{"title":"The Effect of Antisolvent Treatment on the Growth of 2D/3D Tin Perovskite Films for Solar Cells","authors":"Ganghong Min, Robert J. E. Westbrook, Meihuizi Jiang, Margherita Taddei, Ang Li, Thomas Webb, Sanjayan Sathasivam, Amanz Azaden, Robert G. Palgrave, David S. Ginger, Thomas J. Macdonald, Saif A. Haque","doi":"10.1021/acsenergylett.4c02745","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02745","url":null,"abstract":"Antisolvent treatment is used in the fabrication of perovskite films to control grain growth during spin coating. We study widely incorporated aromatic hydrocarbons and aprotic ethers, discussing the origin of their performance differences in 2D/3D Sn perovskite (PEA0.2FA0.8SnI3) solar cells. Among the antisolvents that we screen, diisopropyl ether yields the highest power conversion efficiency in solar cells. We use a combination of optical and structural characterization techniques to reveal that this improved performance originates from a higher concentration of 2D phase, distributed evenly throughout the 2D/3D Sn perovskite film, leading to better crystallinity. This redistribution of the 2D phase, as a result of diisopropyl ether antisolvent treatment, has the combined effect of decreasing the Sn4+ defect density and background hole density, leading to devices with improved open-circuit voltage, short-circuit current, and power conversion efficiency.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"4 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832574","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

Optimized Gas–Liquid Transport via Local Flow Field Management for Efficient Overall Water Splitting

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-17 DOI: 10.1021/acsenergylett.4c02892

Yingjie Ji, Shuyun Yao, Shiyu Wang, Jingxian Li, Yuanming Liu, Kang Ji, Zishan Hou, Xiaojun Wang, Weijie Fu, Lanlan Shi, Jiangzhou Xie, Zhiyu Yang, Yi-Ming Yan

{"title":"Optimized Gas–Liquid Transport via Local Flow Field Management for Efficient Overall Water Splitting","authors":"Yingjie Ji, Shuyun Yao, Shiyu Wang, Jingxian Li, Yuanming Liu, Kang Ji, Zishan Hou, Xiaojun Wang, Weijie Fu, Lanlan Shi, Jiangzhou Xie, Zhiyu Yang, Yi-Ming Yan","doi":"10.1021/acsenergylett.4c02892","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02892","url":null,"abstract":"Electrochemical water splitting is a key technique for sustainable hydrogen production, but its efficiency is often compromised by bubble formation during electrolysis. In this work, we introduce a new electrolyzer design that strategically optimizes gas and liquid flow distributions to facilitate rapid bubble removal, thereby enhancing the electrochemical process. By incorporating a hydrophobic and gas-venting layer, our design significantly shortens the bubble transfer path and reduces the level of accumulation. This advancement results in a voltage reduction of more than 50 mV and a decrease in performance fluctuations exceeding 50% compared with traditional systems. Through detailed optical analyses and finite element simulations, we further elucidate the effects of the gas–liquid transport, enabling high-performance electrolysis with a volumetric current density of 333 mA cm–3 at 1.8 V. These findings underscore the potential of local flow field management in advancing electrolyzer design and other electrochemical systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841542","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

Scalable Electrode Engineering Techniques for Achieving Selective Ethanol Production Using Commercial Copper Catalysts 使用商用铜催化剂实现选择性乙醇生产的可扩展电极工程技术

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2024-12-17 DOI: 10.1021/acsenergylett.4c02916

Haoran Qiu, Lingchun Zeng, Feng Wang, Ya Liu, Liejin Guo

{"title":"Scalable Electrode Engineering Techniques for Achieving Selective Ethanol Production Using Commercial Copper Catalysts","authors":"Haoran Qiu, Lingchun Zeng, Feng Wang, Ya Liu, Liejin Guo","doi":"10.1021/acsenergylett.4c02916","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02916","url":null,"abstract":"In the field of electrochemical CO2 reduction (CO2R), electrode engineering plays a crucial role in modulating the distribution of complex products. Here, based on multiphysics modeling, we demonstrate that CO2R product selectivity varies spatially along the thickness of the catalyst layer of the gas diffusion electrode (GDE). Our calculations indicate that maintaining a moderately low local CO2 concentration around catalytic sites enables optimal ethanol Faradaic efficiency on Cu. We further developed an optimized electrode using commercial Cu nanoparticles with a low catalyst loading of 0.1 mg cm–2. Even under a low CO2 feed concentration of 30%, we achieved a Faradaic efficiency of approximately 65% for ethanol at an industrial-scale current density of–156 mA cm–2 and over 80% for C2+ products, along with a promising cathodic energy efficiency of more than 37% for ethanol. This study serves as a scalable and instructive guide for tuning the local CO2 concentration to achieve optimal production of a single high-selectivity C2+ product.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"52 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142841543","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