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In situ construction of zinc-rich polymeric solid–electrolyte interface for high-performance zinc anode 高性能锌阳极用富锌聚合物固电解质界面的原位构建
eScience Pub Date : 2023-08-01 DOI: 10.1016/j.esci.2023.100153
Kaixuan Xie , Kaixin Ren , Qinghong Wang , Yuxiao Lin , Fengcan Ma , Chuang Sun , Yinwei Li , Xinsheng Zhao , Chao Lai
{"title":"In situ construction of zinc-rich polymeric solid–electrolyte interface for high-performance zinc anode","authors":"Kaixuan Xie ,&nbsp;Kaixin Ren ,&nbsp;Qinghong Wang ,&nbsp;Yuxiao Lin ,&nbsp;Fengcan Ma ,&nbsp;Chuang Sun ,&nbsp;Yinwei Li ,&nbsp;Xinsheng Zhao ,&nbsp;Chao Lai","doi":"10.1016/j.esci.2023.100153","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100153","url":null,"abstract":"<div><p>With their excellent reliability and environmental friendliness, zinc-ion batteries (ZIBs) are regarded as potential energy storage technologies. Unfortunately, their poor cycling durability and low Coulombic effectiveness (CE), driven by dendritic growth and surface passivation on the Zn anode, severely restrict their commercialization. Herein, we describe the <em>in situ</em> construction of a Zn-rich polymeric solid–electrolyte interface (SEI) using polyacrylic acid (PAA) as an electrolyte additive. On the one hand, the PAA SEI layer offers evenly distributed nucleation sites and promotes ion transport, hence suppressing dendrite growth. On the other hand, the SEI layer prevents direct contact between the Zn foil and the electrolyte, thus inhibiting side reactions. Additionally, the robust coordination of PAA with Zn<sup>2+</sup> and the SEI layer's good adherence to the Zn foil provide long-term protection to the Zn anode. As a result, symmetric cells and Zn/V<sub>2</sub>O<sub>5</sub> cells all deliver prolonged cycle life and superior electrochemical efficiency.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49879047","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 11
Electrolyte solvation chemistry to construct an anion-tuned interphase for stable high-temperature lithium metal batteries 构建稳定高温锂金属电池阴离子调谐界面相的电解质溶剂化化学
eScience Pub Date : 2023-08-01 DOI: 10.1016/j.esci.2023.100135
Jiahang Chen , Yang Zhang , Huichao Lu , Juan Ding , Xingchao Wang , Yudai Huang , Huiyang Ma , Jiulin Wang
{"title":"Electrolyte solvation chemistry to construct an anion-tuned interphase for stable high-temperature lithium metal batteries","authors":"Jiahang Chen ,&nbsp;Yang Zhang ,&nbsp;Huichao Lu ,&nbsp;Juan Ding ,&nbsp;Xingchao Wang ,&nbsp;Yudai Huang ,&nbsp;Huiyang Ma ,&nbsp;Jiulin Wang","doi":"10.1016/j.esci.2023.100135","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100135","url":null,"abstract":"<div><p>Lithium metal batteries are regarded as promising alternative next-generation energy storage systems. However, the unstable anode interphase results in dendrite growth and irreversible lithium consumption with low Coulombic efficiency (CE). Herein, we rationally design a Li<sup>+</sup> coordination structure via electrolyte solvation chemistry. Nitrate anions are aggregated in the solvation sheath, even at low concentration in a solvent with moderate solvation ability, which promotes Li<sup>+</sup> desolvation and constructs a nitrate anion-tuned interphase. Meanwhile, a high-donor-number solvent is introduced as an additive to strongly coordinate with Li<sup>+</sup>, which accelerates the ion-transfer kinetics and rate performance. This not only results in micro-sized lithium deposition and a high CE of 99.5% over 3500 ​h, but also enables superior anode stability even under 50% depth plating/stripping and with a lean electrolyte of 3 ​g ​Ah<sup>−1</sup> at 50 ​°C. A lithium–sulfur battery exhibits a prolonged lifespan of 2000 cycles with an average CE of 100%. A full battery using 1x excess lithium exhibits a high capacity near 1600 ​mAh ​g<sub>S</sub><sup>−1</sup> for 100 cycles without capacity loss. Moreover, a 0.55 ​Ah pouch cell delivers a reversible energy density of 423 ​Wh ​kg<sup>−1</sup> based on these electrodes and electrolyte.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49879073","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 2
Steering CO2 electrolysis selectivity by modulating the local reaction environment: An online DEMS approach for Cu electrodes 通过调节局部反应环境来控制CO2电解选择性:Cu电极的在线dem方法
eScience Pub Date : 2023-08-01 DOI: 10.1016/j.esci.2023.100143
Ke Ye , Guiru Zhang , Baoxin Ni , Liang Guo , Chengwei Deng , Xiaodong Zhuang , Changying Zhao , Wen-Bin Cai , Kun Jiang
{"title":"Steering CO2 electrolysis selectivity by modulating the local reaction environment: An online DEMS approach for Cu electrodes","authors":"Ke Ye ,&nbsp;Guiru Zhang ,&nbsp;Baoxin Ni ,&nbsp;Liang Guo ,&nbsp;Chengwei Deng ,&nbsp;Xiaodong Zhuang ,&nbsp;Changying Zhao ,&nbsp;Wen-Bin Cai ,&nbsp;Kun Jiang","doi":"10.1016/j.esci.2023.100143","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100143","url":null,"abstract":"<div><p>Electrochemical CO<sub>2</sub> reduction is a typical surface-mediated reaction, with its reaction kinetics and product distributions largely dependent on the dynamic evolution of reactive species at the cathode–catholyte interface and on the resultant mass transport within the hydrodynamic boundary layer in the vicinity of the cathode. To resolve the complex local reaction environment of branching CO<sub>2</sub> reduction pathways, we here present a differential electrochemical mass spectroscopic (DEMS) approach for Cu electrodes to investigate CO<sub>2</sub> mass transport, the local concentration gradients of buffering anions, and the Cu surface topology effects on CO<sub>2</sub> electrolysis selectivity at a temporal resolution of ∼400 ​ms. As a proof of concept, these tuning knobs were validated on an anion exchange membrane electrolyzer, which delivered a Faradaic efficiency of up to 40.4% and a partial current density of 121 ​mA ​cm<sup>−2</sup> for CO<sub>2</sub>-to-C<sub>2</sub>H<sub>4</sub> valorization. This methodology, which bridges the study of fundamental surface electrochemistry and the upgrading of practical electrolyzer performance, could be of general interest in helping to achieve a sustainable circular carbon economy.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49878984","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 4
The role of machine learning in carbon neutrality: Catalyst property prediction, design, and synthesis for carbon dioxide reduction 机器学习在碳中和中的作用:用于二氧化碳还原的催化剂性能预测、设计和合成
eScience Pub Date : 2023-08-01 DOI: 10.1016/j.esci.2023.100136
Zhuo Wang , Zhehao Sun , Hang Yin , Honghe Wei , Zicong Peng , Yoong Xin Pang , Guohua Jia , Haitao Zhao , Cheng Heng Pang , Zongyou Yin
{"title":"The role of machine learning in carbon neutrality: Catalyst property prediction, design, and synthesis for carbon dioxide reduction","authors":"Zhuo Wang ,&nbsp;Zhehao Sun ,&nbsp;Hang Yin ,&nbsp;Honghe Wei ,&nbsp;Zicong Peng ,&nbsp;Yoong Xin Pang ,&nbsp;Guohua Jia ,&nbsp;Haitao Zhao ,&nbsp;Cheng Heng Pang ,&nbsp;Zongyou Yin","doi":"10.1016/j.esci.2023.100136","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100136","url":null,"abstract":"<div><p>Achieving carbon neutrality is an essential part of responding to climate change caused by the deforestation and over-exploitation of natural resources that have accompanied the development of human society. The carbon dioxide reduction reaction (CO<sub>2</sub>RR) is a promising strategy to capture and convert carbon dioxide (CO<sub>2</sub>) into value-added chemical products. However, the traditional trial-and-error method makes it expensive and time-consuming to understand the deeper mechanism behind the reaction, discover novel catalysts with superior performance and lower cost, and determine optimal support structures and electrolytes for the CO<sub>2</sub>RR. Emerging machine learning (ML) techniques provide an opportunity to integrate material science and artificial intelligence, which would enable chemists to extract the implicit knowledge behind data, be guided by the insights thereby gained, and be freed from performing repetitive experiments. In this perspective article, we focus on recent advancements in ML-participated CO<sub>2</sub>RR applications. After a brief introduction to ML techniques and the CO<sub>2</sub>RR, we first focus on ML-accelerated property prediction for potential CO<sub>2</sub>RR catalysts. Then we explore ML-aided prediction of catalytic activity and selectivity. This is followed by a discussion about ML-guided catalyst and electrode design. Next, the potential application of ML-assisted experimental synthesis for the CO<sub>2</sub>RR is discussed. Finally, we present specific challenges and opportunities, with the aim of better understanding research and advancements in using ML for the CO<sub>2</sub>RR.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49878987","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Efficient air water harvesting of TpPa-1 COFs@LiCl composite driven by solar energy 太阳能驱动下TpPa-1 COFs@LiCl复合材料的高效空气集水
eScience Pub Date : 2023-08-01 DOI: 10.1016/j.esci.2023.100154
Yuxuan Wang , Wen Chen , Jingchao Fu , Yueli Liu
{"title":"Efficient air water harvesting of TpPa-1 COFs@LiCl composite driven by solar energy","authors":"Yuxuan Wang ,&nbsp;Wen Chen ,&nbsp;Jingchao Fu ,&nbsp;Yueli Liu","doi":"10.1016/j.esci.2023.100154","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100154","url":null,"abstract":"<div><p>Adsorbent-assisted air water harvesting (AWH) may help alleviate the current global freshwater scarcity crisis. However, the weak sorption capacity of various adsorbents and the high energy required to release water are two long-standing problems. Herein, we propose a class of green and clean adsorbent, TpPa-1@LiCl composite, whose sorption capacity is greatly improved to 0.37 and 0.80 ​g ​g<sup>−1</sup> under 30% and 90% relative humidity (RH), respectively, and which has excellent stability, showing only a slight decrease (0.79%) after 10 sorption–desorption cycles (1400 ​min). This TpPa-1@LiCl composite can reach equilibrium within 2 ​h and undergo complete desorption in 30 ​min under air mass 1.5 ​G irradiation. A corresponding solar-driven AWH device can complete up to 4 sorption–desorption cycles per day, with each cycle capable of collecting 0.34 ​g ​g<sup>−1</sup> water without additional energy input, which implies TpPa-1@LiCl composite has the potential for achieving sorption-assisted AWH with high efficiency and rapid cycling.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49879048","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 4
Recent advances in cathode catalyst architecture for lithium–oxygen batteries 锂氧电池阴极催化剂结构研究进展
eScience Pub Date : 2023-08-01 DOI: 10.1016/j.esci.2023.100123
Yin Zhou, Shaojun Guo
{"title":"Recent advances in cathode catalyst architecture for lithium–oxygen batteries","authors":"Yin Zhou,&nbsp;Shaojun Guo","doi":"10.1016/j.esci.2023.100123","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100123","url":null,"abstract":"<div><p>Lithium–oxygen (Li–O<sub>2</sub>) batteries have great potential for applications in electric devices and vehicles due to their high theoretical energy density of 3500 ​Wh kg<sup>−1</sup>. Unfortunately, their practical use is seriously limited by the sluggish decomposition of insulating Li<sub>2</sub>O<sub>2</sub>, leading to high OER overpotentials and the decomposition of cathodes and electrolytes. Cathode electrocatalysts with high oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) activities are critical to alleviate high charge overpotentials and promote cycling stability in Li–O<sub>2</sub> batteries. However, constructing catalysts for high OER performance and energy efficiency is always challenging. In this mini-review, we first outline the employment of advanced electrocatalysts such as carbon materials, noble and non-noble metals, and metal–organic frameworks to improve battery performance. We then detail the ORR and OER mechanisms of photo-assisted electrocatalysts and single-atom catalysts for superior Li–O<sub>2</sub> battery performance. Finally, we offer perspectives on future development directions for cathode electrocatalysts that will boost the OER kinetics.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49879072","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 2
Electronic structure regulation of noble metal-free materials toward alkaline oxygen electrocatalysis 无贵金属材料对碱性氧电催化的电子结构调控
eScience Pub Date : 2023-08-01 DOI: 10.1016/j.esci.2023.100141
Xia Wang , Minghao Yu , Xinliang Feng
{"title":"Electronic structure regulation of noble metal-free materials toward alkaline oxygen electrocatalysis","authors":"Xia Wang ,&nbsp;Minghao Yu ,&nbsp;Xinliang Feng","doi":"10.1016/j.esci.2023.100141","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100141","url":null,"abstract":"<div><p>Developing highly efficient, inexpensive catalysts for oxygen electrocatalysis in alkaline electrolytes (i.e., the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER)) is essential for constructing advanced energy conversion techniques (such as electrolyzers, fuel cells, and metal–air batteries). Recent achievements in efficient noble metal-free ORR and OER catalysts make the replacement of conventional noble metal counterparts a realistic possibility. In particular, various electronic structure regulation strategies have been employed to endow these oxygen catalysts with attractive physicochemical properties and strong synergistic effects, providing significant fundamental understanding to advance in this direction. This review article summarizes recently developed electronic structure regulation strategies for three types of noble metal-free oxygen catalysts: transition metal compounds, single-atom catalysts, and metal-free catalysts. We begin by briefly presenting the basic ORR and OER reaction mechanisms, following this with an analysis of the fundamental relationship between electronic structure and intrinsic electrocatalytic activity for the three categories of catalysts. Subsequently, recent advances in electronic structure regulation strategies for noble metal-free ORR and OER catalysts are systematically discussed. We conclude by summarizing the remaining challenges and presenting our outlook on the future for designing and synthesizing noble metal-free oxygen electrocatalysts.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49879075","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 8
Unlocking the charge doping effect in softly intercalated ultrathin ferromagnetic superlattice 解锁软插层超薄铁磁超晶格中的电荷掺杂效应
eScience Pub Date : 2023-06-01 DOI: 10.1016/j.esci.2023.100117
Liang Hu , Bingzhang Yang , Zhipeng Hou , Yangfan Lu , Weitao Su , Lingwei Li
{"title":"Unlocking the charge doping effect in softly intercalated ultrathin ferromagnetic superlattice","authors":"Liang Hu ,&nbsp;Bingzhang Yang ,&nbsp;Zhipeng Hou ,&nbsp;Yangfan Lu ,&nbsp;Weitao Su ,&nbsp;Lingwei Li","doi":"10.1016/j.esci.2023.100117","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100117","url":null,"abstract":"<div><p>The electrolyte-assisted exfoliation strategy is widely employed to synthesize ultrathin two-dimensional (2D) materials. Yet, spins in 2D magnets are susceptible to the electrolyte due to the underlying charge doping effect. Hence, it is crucial to understand and trace the doping process during the delamination of 2D magnets. Taking the prototype Fe<sub>3</sub>GeTe<sub>2</sub>, we utilized soft organic cations to exfoliate the bulk and obtain a freestanding organic–inorganic hybrid superlattice with a giant electron doping effect as high as 6.9 ​× ​10<sup>14</sup>/cm<sup>2</sup> (∼1.15 electrons per formula unit). A remarkable ferromagnetic transition exceeding 385 ​K was revealed in these superlattices, together with unique anisotropic saturation magnetization. The doping enhanced the in-plane electron–phonon coupling and thus optimized originally poor indirect double-exchange scenario for spin electrons. The emerging vertical magnetization shift phenomenon served to evaluate the uniformity of charge doping. The above findings provide a new perspective for understanding the role of parasitic charge in 2D magnetism.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49884204","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Modulating single-molecule charge transport through external stimulus 通过外部刺激调节单分子电荷输运
eScience Pub Date : 2023-06-01 DOI: 10.1016/j.esci.2023.100115
Qi Zou , Jin Qiu , Yaping Zang , He Tian , Latha Venkataraman
{"title":"Modulating single-molecule charge transport through external stimulus","authors":"Qi Zou ,&nbsp;Jin Qiu ,&nbsp;Yaping Zang ,&nbsp;He Tian ,&nbsp;Latha Venkataraman","doi":"10.1016/j.esci.2023.100115","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100115","url":null,"abstract":"<div><p>Understanding and tuning charge transport over a single molecule is a fundamental topic in molecular electronics. Single-molecule junctions composed of individual molecules attached to two electrodes are the most common components built for single-molecule charge transport studies. During the past two decades, rapid technical and theoretical advances in single-molecule junctions have increased our understanding of the conductance properties and functions of molecular devices. In this perspective article, we introduce the basic principles of charge transport in single-molecule junctions, then give an overview of recent progress in modulating single-molecule transport through external stimuli such as electric field and potential, light, mechanical force, heat, and chemical environment. Lastly, we discuss challenges and offer views on future developments in molecular electronics.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49884199","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A green repair pathway for spent spinel cathode material: Coupled mechanochemistry and solid-phase reactions 废尖晶石正极材料的绿色修复途径:机械化学与固相反应的耦合
eScience Pub Date : 2023-06-01 DOI: 10.1016/j.esci.2023.100110
Jiao Lin , Xu Chen , Ersha Fan , Xiaodong Zhang , Renjie Chen , Feng Wu , Li Li
{"title":"A green repair pathway for spent spinel cathode material: Coupled mechanochemistry and solid-phase reactions","authors":"Jiao Lin ,&nbsp;Xu Chen ,&nbsp;Ersha Fan ,&nbsp;Xiaodong Zhang ,&nbsp;Renjie Chen ,&nbsp;Feng Wu ,&nbsp;Li Li","doi":"10.1016/j.esci.2023.100110","DOIUrl":"https://doi.org/10.1016/j.esci.2023.100110","url":null,"abstract":"<div><p>A way of directly repairing spent lithium-ion battery cathode materials is needed in response to environmental pollution and resource depletion. In this work, we report a green repair method involving coupled mechanochemistry and solid-state reactions for spent lithium-ion batteries. During the ball-milling repair process, an added manganese source enters into the degraded LiMn<sub>2</sub>O<sub>4</sub> (LMO) crystal structure in order to fill the Mn vacancies formed by Mn deficiency due to the Jahn–Teller effect, thereby repairing the LMO's chemical composition. An added carbon source acts not only as a lubricant but also as a conductor to improve the material's electrical conductivity. Meanwhile, mechanical force reduces the crystal size of the LMO particles, increasing the amount of active sites for electrochemical reactions. Jahn–Teller distortion is successfully suppressed by cation disorder in the LMO material. The cycling stability and rate performance of the repaired cathode material are thereby greatly improved, with the discharge specific capacity being more than twice that of commercial LMO. The proposed solid-state mechanochemical in situ repair process, which is safe for the environment and simple to use, may be extended to the repair of other waste materials without consuming highly acidic or alkaline chemical reagents.</p></div>","PeriodicalId":100489,"journal":{"name":"eScience","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49883647","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
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