Pub Date : 2024-06-27DOI: 10.1021/acsenergylett.4c01244
Wen Chen, Haotian Qu, Ruyu Shi, Junxiong Wang, Haocheng Ji, Zhaofeng Zhuang, Jun Ma, Di Tang, Junfeng Li, Jie Tang, Guanjun Ji, Xiao Xiao, Yanfei Zhu, Guangmin Zhou
Recycling the graphite anode is essential for both environmental protection and resource sustainability in lithium-ion batteries. Current recycling strategies emphasize closed-loop recovery but ignore the potential for value-added utilization. Herein, we present an upcycling strategy that converts spent graphite into fast-charging graphite. By creating an isotropic ion transport pathway on the surface of spent graphite and utilizing the fast ion migration channel inherent in the bulk’s defect structure, a direct upgrade of spent graphite for fast charging is achieved. A proposed structure model, derived from spent graphite, shows improved fast-charging performance at the particle and electrode levels. Regenerated graphite demonstrates a high specific capacity of 220 mAh g–1 at 4C, approximately 2.8 times higher than that of commercial graphite (80 mAh g–1), with 73% of capacity retention after 300 cycles. This work provides fundamental insights into upcycling spent graphite, featuring short production processes and great economic and environmental benefits.
回收石墨负极对于锂离子电池的环境保护和资源可持续性至关重要。目前的回收策略强调闭环回收，但忽视了增值利用的潜力。在此，我们提出了一种将废石墨转化为快速充电石墨的升级再循环策略。通过在废石墨表面建立各向同性的离子传输通道，并利用块体缺陷结构中固有的快速离子迁移通道，实现了废石墨的直接升级，从而实现快速充电。根据废石墨提出的结构模型显示，颗粒和电极层面的快速充电性能得到了改善。再生石墨在 4C 时的比容量高达 220 mAh g-1，是商用石墨（80 mAh g-1）的约 2.8 倍，300 次循环后的容量保持率为 73%。这项工作为废石墨的升级再循环提供了基本见解，其特点是生产流程短，具有巨大的经济和环境效益。
{"title":"Upcycling Spent Graphite into Fast-Charging Anode Materials through Interface Regulation","authors":"Wen Chen, Haotian Qu, Ruyu Shi, Junxiong Wang, Haocheng Ji, Zhaofeng Zhuang, Jun Ma, Di Tang, Junfeng Li, Jie Tang, Guanjun Ji, Xiao Xiao, Yanfei Zhu, Guangmin Zhou","doi":"10.1021/acsenergylett.4c01244","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01244","url":null,"abstract":"Recycling the graphite anode is essential for both environmental protection and resource sustainability in lithium-ion batteries. Current recycling strategies emphasize closed-loop recovery but ignore the potential for value-added utilization. Herein, we present an upcycling strategy that converts spent graphite into fast-charging graphite. By creating an isotropic ion transport pathway on the surface of spent graphite and utilizing the fast ion migration channel inherent in the bulk’s defect structure, a direct upgrade of spent graphite for fast charging is achieved. A proposed structure model, derived from spent graphite, shows improved fast-charging performance at the particle and electrode levels. Regenerated graphite demonstrates a high specific capacity of 220 mAh g<sup>–1</sup> at 4C, approximately 2.8 times higher than that of commercial graphite (80 mAh g<sup>–1</sup>), with 73% of capacity retention after 300 cycles. This work provides fundamental insights into upcycling spent graphite, featuring short production processes and great economic and environmental benefits.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141463627","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}
Pub Date : 2024-06-27DOI: 10.1021/acsenergylett.4c01292
Fuzong Xu, Jiang Liu, Lujia Xu, Arsalan Razzaq, Xuechun Zhang, Erkan Aydin, Stefaan De Wolf
The first four-terminal perovskite/perovskite/silicon triple-junction tandem solar cells are reported, with the device structure comprising a perovskite single-junction top cell and monolithic perovskite/silicon tandem bottom cell, yielding a 31.5% power conversion efficiency. Key to this result was the hole-transporting-layer engineering of the top cell, which led to enhanced performance and reproducibility of the 1 cm2 semitransparent inverted perovskite solar cells.
{"title":"Four-Terminal Perovskite/Perovskite/Silicon Triple-Junction Tandem Solar Cells with over 30% Power Conversion Efficiency","authors":"Fuzong Xu, Jiang Liu, Lujia Xu, Arsalan Razzaq, Xuechun Zhang, Erkan Aydin, Stefaan De Wolf","doi":"10.1021/acsenergylett.4c01292","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01292","url":null,"abstract":"The first four-terminal perovskite/perovskite/silicon triple-junction tandem solar cells are reported, with the device structure comprising a perovskite single-junction top cell and monolithic perovskite/silicon tandem bottom cell, yielding a 31.5% power conversion efficiency. Key to this result was the hole-transporting-layer engineering of the top cell, which led to enhanced performance and reproducibility of the 1 cm<sup>2</sup> semitransparent inverted perovskite solar cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141463668","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}
Pub Date : 2024-06-26DOI: 10.1021/acsenergylett.4c01061
Xiangyu Li, Bachir El Fil, Buxuan Li, Gustav Graeber, Adela C. Li, Yang Zhong, Mohammed Alshrah, Chad T. Wilson, Emily Lin
Water scarcity remains a grand challenge across the globe. Sorption-based atmospheric water harvesting (SAWH) is an emerging and promising solution for water scarcity, especially in arid and noncoastal regions. Traditional approaches to AWH such as fog harvesting and dewing are often not applicable in an arid environment (<30% relative humidity (RH)), whereas SAWH has demonstrated great potential to provide fresh water under a wide range of climate conditions. Despite advances in materials development, most demonstrated SAWH devices still lack sufficient water production. In this work, we focus on the adsorption bed design to achieve high water production, multicyclic operation, and a compact form factor (high material loading per heat source contact area). The modeling efforts and experimental validation illustrate an optimized design space with a fin-array adsorption bed enabled by high-density waste heat, which promises 5.826 Lwater kgsorbent–1 day–1 at 30% RH within a compact 1 L adsorbent bed and commercial adsorbent materials.
{"title":"Design of a Compact Multicyclic High-Performance Atmospheric Water Harvester for Arid Environments","authors":"Xiangyu Li, Bachir El Fil, Buxuan Li, Gustav Graeber, Adela C. Li, Yang Zhong, Mohammed Alshrah, Chad T. Wilson, Emily Lin","doi":"10.1021/acsenergylett.4c01061","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01061","url":null,"abstract":"Water scarcity remains a grand challenge across the globe. Sorption-based atmospheric water harvesting (SAWH) is an emerging and promising solution for water scarcity, especially in arid and noncoastal regions. Traditional approaches to AWH such as fog harvesting and dewing are often not applicable in an arid environment (<30% relative humidity (RH)), whereas SAWH has demonstrated great potential to provide fresh water under a wide range of climate conditions. Despite advances in materials development, most demonstrated SAWH devices still lack sufficient water production. In this work, we focus on the adsorption bed design to achieve high water production, multicyclic operation, and a compact form factor (high material loading per heat source contact area). The modeling efforts and experimental validation illustrate an optimized design space with a fin-array adsorption bed enabled by high-density waste heat, which promises 5.826 L<sub>water</sub> kg<sub>sorbent</sub><sup>–1</sup> day<sup>–1</sup> at 30% RH within a compact 1 L adsorbent bed and commercial adsorbent materials.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461566","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}
Pub Date : 2024-06-26DOI: 10.1021/acsenergylett.4c01215
Xinlin Li, Xianyang Wu, Hieu A. Doan, Zhenzhen Yang, Rachid Amine, Matthew Li, M. Victoria Bracamonte, Chi-Cheung Su, Khalil Amine
Judicious selection of the optimal fluorobenzene (FB) as a nonsolvating cosolvent for lithium metal batteries (LMBs) is reported. We found the key correlation between FB structures and cycling stabilities of cells: increased fluorine substitution of FBs results in higher anodic stability but at the expense of reduced reductive stability, and FBs containing three or more fluorine atoms exhibit insufficient anodic stability in the electrolyte system comprised of fluoroethylene carbonate (FEC) and ethyl methyl carbonate (EMC). More importantly, FBs with higher acidity (lower pKa) due to protons located between two adjacent fluorine atoms tend to be more susceptible to side reactions during cycling. Our results indicate that difluorobenzenes with no “acidic” proton (DFB2 and DFB4) have emerged as the optimal choice with the desired redox stability in high-voltage LMBs. Nuclear magnetic resonance and X-ray photoelectron spectroscopy confirmed these findings, providing guidance for selecting the most suitable FB variants as nonsolvating cosolvents for high-voltage LMBs.
{"title":"Acidity-Governed Rules in the Electrochemical Performance of Fluorinated Benzenes for High-Voltage Lithium Metal Batteries","authors":"Xinlin Li, Xianyang Wu, Hieu A. Doan, Zhenzhen Yang, Rachid Amine, Matthew Li, M. Victoria Bracamonte, Chi-Cheung Su, Khalil Amine","doi":"10.1021/acsenergylett.4c01215","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01215","url":null,"abstract":"Judicious selection of the optimal fluorobenzene (FB) as a nonsolvating cosolvent for lithium metal batteries (LMBs) is reported. We found the key correlation between FB structures and cycling stabilities of cells: increased fluorine substitution of FBs results in higher anodic stability but at the expense of reduced reductive stability, and FBs containing three or more fluorine atoms exhibit insufficient anodic stability in the electrolyte system comprised of fluoroethylene carbonate (FEC) and ethyl methyl carbonate (EMC). More importantly, FBs with higher acidity (lower p<i>K</i><sub>a</sub>) due to protons located between two adjacent fluorine atoms tend to be more susceptible to side reactions during cycling. Our results indicate that difluorobenzenes with no “acidic” proton (DFB2 and DFB4) have emerged as the optimal choice with the desired redox stability in high-voltage LMBs. Nuclear magnetic resonance and X-ray photoelectron spectroscopy confirmed these findings, providing guidance for selecting the most suitable FB variants as nonsolvating cosolvents for high-voltage LMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461564","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}
Pub Date : 2024-06-25DOI: 10.1021/acsenergylett.4c01603
Anton A. Samoylov, Matthew Dailey, Yanan Li, Patrick J. Lohr, Sean Raglow, Adam D. Printz
Pages 2101 and 2104. The authors discovered an error in the calculation of the biaxial moduli derived from the slopes of the stress curves in Figure S1. In our calculations of the moduli using eq 2, we inadvertently had inverted the slopes of the linear elastic region (i.e., we used d𝑇d𝜎
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