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An efficient recycling strategy to eliminate the residual“impurities”while heal the damaged structure of spent graphite anodes

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Green Energy & Environment 2024年第6期9卷 1027-1034页

作者： Dan Yang Ying Yang Haoran Du Yongsheng Ji Mingyuan Ma Yujun Pan Xiaoqun Qi Quan Sun Kaiyuan Shi long qie Institute of New Energy for Vehicles School of Materials Science and EngineeringTongji UniversityShanghai201804China State Key Laboratory of Material Processing and Die&Mold Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan430074China Shuangdeng Group Co. Ltd.Taizhou225500China School of Materials Science and Engineering Sun Yat-Sen UniversityGuangzhou510275China

The recycling of graphite from spent lithium-ion batteries(LIBs)is overlooked due to its relatively low added value and the lack of efficient recovering methods.To reuse the spent graphite anodes,we need to eliminate their useless components(mainly the degraded solid electrolyte interphase,SEI)and reconstruct their damaged structure.Herein,a facile and efficient strategy is proposed to recycle the spent graphite on the basis of the careful investigation of the composition of the cycled graphite anodes and the rational design of the regeneration processes.The regenerated graphite,which is revitalized by calcination treatment and acid leaching,delivers superb rate performance and a high specific capacity of 370 mAh g^(-1)(~99% of its theoretical capacity)after 100 cycles at 0.1 C,superior to the commercial graphite anodes.The improved electrochemical performance could be attributed to unchoked Li^(+) transport channels and enhanced charge transfer reaction due to the effective destruction of the degraded SEI and the full recovery of the damaged structure of the spent graphite.This work clarifies that the electrochemical performance of the regenerated graphite could be deteriorated by even a trace amount of the residual“impurity”and provides a facile method for the efficient regeneration of graphite anodes.

关键词： Graphite Anode Regeneration Solid electrolyte interphase Spent lithium-ion battery

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Targeted regeneration and upcycling of spent graphite by defect‐driven tin nucleation

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Carbon Energy 2024年第4期6卷 91-103页

作者： Zhiheng Cheng Zhiling Luo Hao Zhang Wuxing Zhang Wang Gao Yang Zhang long qie Yonggang Yao Yunhui Huang Kun Kelvin Fu State Key Laboratory of Materials Processing and Die&Mould Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhanChina Key Laboratory of Automobile Materials(Jilin University) Ministry of EducationDepartment of Materials Science and EngineeringJilin UniversityChangchunChina Electronic Materials Research Laboratory(Key Lab of Education Ministry) School of Electronic and Information Engineeringand Instrumental Analysis CenterXi'an Jiaotong UniversityXi'anChina Department of Mechanical Engineering University of DelawareNewarkUSA

The recycling of spent batteries has become increasingly important owing to their wide applications,abundant raw material supply,and sustainable development.Compared with the degraded cathode,spent anode graphite often has a relatively intact structure with few defects after long cycling.Yet,most spent graphite is simply burned or discarded due to its limited value and inferior performance on using conventional recycling methods that are complex,have low efficiency,and fail in performance restoration.Herein,we propose a fast,efficient,and“intelligent”strategy to regenerate and upcycle spent graphite based on defect‐driven targeted remediation.Using Sn as a nanoscale healant,we used rapid heating(~50 ms)to enable dynamic Sn droplets to automatically nucleate around the surface defects on the graphite upon cooling owing to strong binding to the defects(~5.84 eV/atom),thus simultaneously achieving Sn dispersion and graphite remediation.As a result,the regenerated graphite showed enhanced capacity and cycle stability(458.9 mAh g^(−1) at 0.2 A g^(−1) after 100 cycles),superior to those of commercial graphite.Benefiting from the self‐adaption of Sn dispersion,spent graphite with different degrees of defects can be regenerated to similar structures and performance.EverBatt analysis indicates that targeted regeneration and upcycling have significantly lower energy consumption(~99%reduction)and near‐zero CO2 emission,and yield much higher profit than hydrometallurgy,which opens a new avenue for direct upcycling of spend graphite in an efficient,green,and profitable manner for sustainable battery manufacture.

关键词： battery recycling spent graphite targeted regeneration upcycling graphite

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A Stretchable Ionic Conductive Elastomer for High-Areal-Capacity Lithium-Metal Batteries

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Energy & Environmental Materials 2022年第1期5卷 337-343页

作者： Kejia Li Zhenglu Zhu Ruirui Zhao Haoran Du Xiaoqun Qi Xiaobin Xu long qie Institute of New Energy for Vehicles School of Materials Science and EngineeringTongji UniversityShanghai 201804China

Developing high-areal-capacity and dendrite-free lithium(Li)anodes is of significant importance for the practical applications of the Li-metal secondary batteries.Herein,an effective strategy to stabilize the high-arealcapacity Li electrodeposition by modifying the Li metal with a stretchable ionic conductive elastomer(ICE)is demonstrated.The ICE layer prepared via an instant photocuring process shows a promising Li^(+)-ion conductivity at room temperature.When being used in Li-metal batteries,the thin ICE coating(~0.27μm)acts as both a stretchable constraint to minimize the Li loss and a protective layer to facilitate the uniform flux of Li ions.With this ICE-modifying strategy,the reversibility and cyclability of the Li anodes under high-areal-capacity condition in carbonate electrolyte are significantly improved,leading to a stable Li stripping/plating for 500 h at an ultrahigh areal capacity of 20 mAh cm^(-2)in commercial carbonate electrolyte.When coupled with industry-level thick LiFePO;electrodes(20.0 mg cm^(-2)),the cells with ICE-Li anodes show significantly enhanced rate and cycling capability.

关键词： high areal capacity ionic conductive elastomer lithium anode lithium-metal battery protective layer

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Demystifying the Salt‑Induced Li Loss:A Universal Procedure for the Electrolyte Design of Lithium‑Metal Batteries

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Nano-Micro Letters 2023年第12期15卷 310-319页

作者： Zhenglu Zhu Xiaohui Li Xiaoqun Qi Jie Ji Yongsheng Ji Ruining Jiang Chaofan Liang Dan Yang Ze Yang long qie Yunhui Huang State Key Laboratory of Material Processing and Die and Mold Technology School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiPeople’s Republic of China Institute of New Energy for Vehicles School of Materials Science and EngineeringTongji UniversityShanghai 201804People’s Republic of China Institute of Nanoscience and Nanotechnology School of Physical Science and TechnologyCentral China Normal UniversityWuhan 430079People’s Republic of China

Lithium(Li)metal electrodes show significantly different reversibility in the electrolytes with different salts.However,the understanding on how the salts impact on the Li loss remains unclear.Herein,using the electrolytes with different salts(e.g.,lithium hexafluorophosphate(LiPF_(6)),lithium difluoro(oxalato)borate(LiDFOB),and lithium bis(fluorosulfonyl)amide(LiFSI))as examples,we decouple the irreversible Li loss(SEI Li^(+)and“dead”Li)during cycling.It is found that the accumulation of both SEI Li^(+)and“dead”Li may be responsible to the irreversible Li loss for the Li metal in the electrolyte with LiPF_(6)salt.While for the electrolytes with LiDFOB and LiFSI salts,the accumulation of“dead”Li predominates the Li loss.We also demonstrate that lithium nitrate and fluoroethylene carbonate additives could,respectively,function as the“dead”Li and SEI Li^(+)inhibitors.Inspired by the above understandings,we propose a universal procedure for the electrolyte design of Li metal batteries(LMBs):(i)decouple and find the main reason for the irreversible Li loss;(ii)add the corresponding electrolyte additive.With such a Li-loss-targeted strategy,the Li reversibility was significantly enhanced in the electrolytes with 1,2-dimethoxyethane,triethyl phosphate,and tetrahydrofuran solvents.Our strategy may broaden the scope of electrolyte design toward practical LMBs.

关键词： Li loss Universal guideline Electrolyte design Li reversibility

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A long-life and safe lithiated graphite-selenium cell with competitive gravimetric and volumetric energy densities

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Journal of Energy Chemistry 2021年第9期30卷 556-563页

作者： Xiaoqun Qi Qiang Jin Fengyi Yang Ruining Jiang Quan Sun long qie Yunhui Huang Institute of New Energy for Vehicles School of Materials Science and EngineeringTongji UniversityShanghai 201804China

Lithium-selenium(Li-Se) battery is a promising system with high theoretical gravimetric and volumetric energy densities, while its long-term cyclability is hard to realize, especially when a practical Se cathode with high Se content, high Se loading, and high density is employed. The main obstacles are the sluggish conversion kinetics of the dense Se cathodes and the continuous deterioration of the Li-metal anodes.Here, by introducing an acetonitrile(AN)-based electrolyte and replacing the Li electrode with a lithiated graphite, we successfully build a hybrid conversion-intercalation system using a high-content(80 wt%),decent-loading(3.0 mg cm^(-2)), and low-porosity(44%) Se cathode. The as-designed lithiated graphite||Se(LG||Se) cell demonstrated a high Se utilization(97.4%), a long cycle life(3000 cycles), and an ultrahigh average Coulombic efficiency(99.98%). The cell also works well under lean-electrolyte(2 l L mg^(-1)) condition and shows outstanding safety performance in the nail-penetrating test. The combination affords the competitive comprehensive performances, including high volumetric and gravimetric energy densities, long cycling life, and superb safety of the LG||Se cell. In addition, with a newly-designed threeelectrode pouch cell, the lithiation of the graphite anodes could be done with an in-situ lithiation process,indicating the high potential of the as-proposed LG||Se cell for the practical applications.

关键词： Conversion-intercalation Acetonitrile electrolyte Se cathode Lithiated graphite Energy density

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Design of Lattice Structures Using Local Relative Density Mapping Method

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Chinese Journal of Mechanical Engineering 2018年第5期31卷 110-118页

作者： Guo-Hua Song Shi-Kai Jing Fang-Lei Zhao Ye-Dong Wang Hao Xing long-Fei qie Beijing Xinghang Mechanical-electrical Equipment Co.Ltd. Beijing 100074 China School of Mechanical Engineering Beijing Institute of Technology Beijing 100081 China

In order to solve the problem of substantial computational resources of lattice structure during optimization, a local relative density mapping(LRDM) method is proposed. The proposed method uses solid isotropic microstructures with penalization to optimize a model at the macroscopic scale. The local relative density information is obtained from the topology optimization result. The contour lines of an optimized model are extracted using a density contour approach, and the triangular mesh is generated using a mesh generator. A local mapping relationship between the elements’ relative density and the struts’ relative cross?sectional area is established to automatically determine the diameter of each individual strut in the lattice structures. The proposed LRDM method can be applied to local finite element meshes and local density elements, but it is also suitable for global ones. In addition, some cases are con?sidered in order to test the e ectiveness of the LRDM method. The results show that the solution time of the LRDM is lower than the RDM method by approximately 50%. The proposed method provides instructions for the design of more complex lattice structures.

关键词： Lattice structures Local relative density mapping Topology optimization Additive manufacturing

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高安全锂离子电池复合集流体的界面强化

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物理化学学报 2023年第2期39卷 81-92页

作者：汪茹刘志康严超伽龙黄云辉同济大学材料科学与工程学院上海201804 华中科技大学材料科学与工程学院材料成形与模具技术国家重点实验室武汉430074 南京同宁新材料研究院有限公司南京211161 浙江柔震科技有限公司浙江嘉兴314499

面向高能量密度电池的高比容量三元正极材料的应用,使锂离子电池更容易发生热失控,这不仅降低了其安全性,也限制了锂离子电池的进一步发展。如何在提高能量密度的同时保证电池的安全性是亟待解决的问题。以绝缘高分子薄膜为支撑基材,两... 详细信息

面向高能量密度电池的高比容量三元正极材料的应用,使锂离子电池更容易发生热失控,这不仅降低了其安全性,也限制了锂离子电池的进一步发展。如何在提高能量密度的同时保证电池的安全性是亟待解决的问题。以绝缘高分子薄膜为支撑基材,两侧沉积金属层得到了具有夹芯结构的铝复合集流体能有效保证电池在针刺条件下的安全性,且更轻的复合集流体的使用能进一步提高电池能量密度。但高分子基材与铝金属层之间界面结合力较差,这会导致复合集流体在高温电解液浸泡中发生脱层现象,从而影响其在电池中的使用。本研究采用聚对苯二甲酸乙二醇酯(PET)作为支撑基材,通过在铝金属镀层与高分子基材之间引入氧化物中间层,有效地增强了金属与高分子基材之间的界面结合力,提升复合集流体的电解液兼容性。此外,复合集流体良好的机械性能使其能很好地兼容现有的电池制备技术,利用其制备的软包电池表现出与使用传统铝箔为集流体的电池相当的电化学性能。进一步的针刺测试表明,复合集流体能有效阻止锂电池在针刺过程中的热失控,显著改善了电池的安全性能。

关键词：锂离子电池复合集流体界面强化氧化物强化层电解液兼容性

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Chinese expert consensus on diagnosis and treatment of anal intraepithelial neoplasia

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Gynecology and Obstetrics Clinical Medicine 2024年第1期4卷 3-10页

作者： Yanyun Li Hongwei Zhang Qing Cong Mingzhu Li Hui Bi Yun Zhao Zhixue You Qi Zhou Li Geng Mingrong qie Fanghui Zhao Linhong Wang Beihua Kong Ding Ma long Sui Lihui Wei Hospital and Institute of Obstetrics and Gynecology Fudan UniversityShanghaiChina Department of Obstetrics and Gynecology Peking University People's HospitalBeijingChina Department of Obstetrics and Gynecology Peking University First HospitalBejingChina Department of Obstetrics and Gynecology Jiangsu Province People's Hospital and Nanjing Medical University First Affiliated HospitalNanjingJiangsuChina Chongqing University Cancer Hospital ChongqingChina Department of Obstetrics and Gynecology Peking University Third HospitalBejingChina Sichuan University West China Second University Hospital ChengduSichuanChina National Center for Chronic and Non-communicable Disease Control and Prevention Chinese Center for Disease Control and PreventionBeijingChina Department of Obstetrics and Gynecology Qilu Hospital of Shandong UniversityJinanShandongChina Department of Obstetrics and Gynecology Tongji HospitalTongji Medical Cllege of HUSTWuhanChina

Anal high-grade squamous intraepithelial lesion(HSIL)refers to the precancerous lesions of anal squamous cell carcinoma(ASCC).Anal cancer is often asymptomatic in its early stage.

关键词： diagnosis squamous intraepithelial

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对“综合高中”作为一个原型范畴的诠释——基于比较研究的视角

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外国教育研究 2024年第3期51卷 17-32页

作者：曾凤琴郄海霞天津大学教育学院天津300350

作为高中教育“模式求解”的重要选择,我国发展综合高中的教育改革之所以长期以来步履维艰,与对“什么是综合高中”的认识一直模糊不清高度相关。其实,综合高中主要是一个原型范畴而非特征范畴,给它下一个精确的定义不仅非常困难,而且... 详细信息

作为高中教育“模式求解”的重要选择,我国发展综合高中的教育改革之所以长期以来步履维艰,与对“什么是综合高中”的认识一直模糊不清高度相关。其实,综合高中主要是一个原型范畴而非特征范畴,给它下一个精确的定义不仅非常困难,而且也没有必要。美国的综合高中是“综合高中”范畴的原型,是集合了该范畴成员最多特征的清楚的样本,具有教育对象的大众性、培养目标的三维性、教育分流的内部性、课程设置的综合性、学校规模的超大性等特征。英国、日本等其他国家的综合高中虽然都具有综合高中的“家族相似性”,但其形态各异并呈现出动态性,有的属于“综合高中”的典型成员,有的是非典型成员,还有的则具有边界的模糊性。综合高中没有也不应该有固定不变的统一模式,各国应根据具体国情和变动不居的时代需要建设和发展“自己的”综合高中。我国综合高中的发展要走出困境,应立足于有效解决高中教育普职“二元分离”问题,基于社会工程思维重建综合高中实践模式。

关键词：综合高中原型范畴多样化动态性

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肝细胞癌双硫死亡相关lncRNA预后模型构建和功能机制探索

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标记免疫分析与临床 2024年第6期31卷 1144-1150页

作者：刘艺涵崔龙李欣客蕊黑龙江中医药大学黑龙江哈尔滨150000 齐齐哈尔市中医院肿瘤科黑龙江齐齐哈尔161000 齐齐哈尔医学院附属四院黑龙江齐齐哈尔161000 黑龙江中医药大学附属第一医院老年病科黑龙江哈尔滨150000

目的探索双硫死亡相关长链非编码RNA(lncRNA),进一步构建风险预测模型,以期为肝细胞癌的预后评估及个体化治疗提供新的生物标志物。方法从TCGA数据平台中下载肝细胞癌转录组数据及临床数据,运用皮尔森相关分析筛选出双硫死亡相关lncRNA... 详细信息

目的探索双硫死亡相关长链非编码RNA(lncRNA),进一步构建风险预测模型,以期为肝细胞癌的预后评估及个体化治疗提供新的生物标志物。方法从TCGA数据平台中下载肝细胞癌转录组数据及临床数据,运用皮尔森相关分析筛选出双硫死亡相关lncRNA。通过多种算法构建预测模型。采用单因素和多因素Cox回归、Kaplan-Meier生存曲线、ROC曲线、DCA决策曲线以及列线图对预后模型进行效能评估和验证。计算每例患者的风险评分,根据评分中位数将患者分为低风险组和高风险组,进行免疫逃逸(TIDE)、免疫检查点、m6A修饰基因相关性分析以及药物敏感性分析,通过基因突变、基因集富集分析(GSEA)对其生物学特征进行评价。结果本研究共鉴定了5个双硫死亡相关lncRNAs并据此构建风险预测模型。生存分析显示高风险组患者总生存期显著低于低风险组(P<0.001)。该模型的1、3、5年生存预测AUC值分别为0.773、0.725和0.679。单因素、多因素Cox回归证实了该模型的独立预后价值(P<0.001)。列线图内部验证显示模型预测的可信度较好。高低风险组在免疫逃逸潜能评分、关键免疫检查点和m6A修饰基因表达水平、以及对常用HCC治疗药物的耐药性上均表现出显著差异。结论本研究构建的双硫死亡相关lncRNAs预后模型具有良好的预测准确性,可作为新的生物标志物,评估HCC患者的生存预后和免疫逃逸倾向,为临床决策提供有价值的参考。

关键词：肝细胞癌双硫死亡长链非编码RNA 预测模型

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