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Localized-domains staging structure and evolution in lithiated graphite

Carbon Energy 2023年第1期5卷 144-153页

作者： Suting Weng Siyuan Wu Zepeng Liu Gaojing Yang Xiaozhi Liu Xiao Zhang Chu Zhang Qiuyan Liu Yao Huang Yejing Li Mehmet NAteş Dong Su Lin Gu Hong Li Liquan Chen Ruijuan Xiao Zhaoxiang Wang Xuefeng Wang Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijingChina School of Physical Sciences University of Chinese Academy of SciencesBeijingChina College of Materials Science and Opto-Electronic Technology University of Chinese Academy of SciencesBeijingChina Energy Storage Division TÜBİTAK Rail Transport Technologies InstituteTÜBİTAK Gebze CampusGebzeKocaeliTurkey Tianmu Lake Institute of Advanced Energy Storage Technologies Co. Ltd.LiyangJiangsuChina

Intercalation provides to the host materials a means for controlled variation of many physical/chemical properties and dominates the reactions in metal‐ion batteries.Of particular interest is the graphite intercalation compounds with intriguing staging structures,which however are still unclear,especially in their nanostructure and dynamic transition mechanism.Herein,the nature of the staging structure and evolution of the lithium(Li)‐intercalated graphite was revealed by cryogenic‐transmission electron microscopy and other methods at the nanoscale.The intercalated Li‐ions distribute unevenly,generating local stress and dislocations in the graphitic structure.Each staging compound is found macroscopically ordered but microscopically inhomogeneous,exhibiting a localized‐domains structural model.Our findings uncover the correlation between the long‐range ordered structure and short‐range domains,refresh the insights on the staging structure and transition of Li‐intercalated/deintercalated graphite,and provide effective ways to enhance the reaction kinetic in rechargeable batteries by defect engineering.

关键词： cryogenic-transmission electron microscopy(cryo-TEM) graphite intercalation compounds lithiated graphite localized-domains structural model staging structures

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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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Surplus energy utilization of spent lithium-ion batteries for high-profit organolithiums

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Carbon Energy 2023年第6期5卷 11-20页

作者： Jian Lu Yun Zhao Yuqiong Kang Chenglei Li Yawen Liu Liguang Wang Hao Du Meicen Fan Yunan Zhou John Wozny Tao Li Naser Tavajohi Feiyu Kang Baohua Li Shenzhen Key Laboratory on Power Battery Safety Tsinghua Shenzhen International Graduate School(SIGS)Shenzhen Geim Graphene CenterShenzhenChina College of Chemical and Biological Engineering Zhejiang UniversityHangzhouChina Institute of Zhejiang University QuzhouChina Department of Chemistry and Biochemistry Northern Illinois UniversityDeKalbIllinoisUSA Department of Chemistry UmeåUniversityUmeåSweden

It is challenging to efficiently and economically recycle many lithium-ion batteries(LIBs)because of the low valuation of commodity metals and materials,such as LiFePO_(4).There are millions of tons of spent LIBs where the barrier to recycling is economical,and to make recycling more feasible,it is required that the value of the processed recycled material exceeds the value of raw commodity materials.The presented research illustrates improved profitability and economics for recycling spent LIBs by utilizing the surplus energy in lithiated graphite to drive the preparation of organolithiums to add value to the recycled lithium materials.This study methodology demonstrates that the surplus energy of lithiated graphite obtained from spent LIBs can be utilized to prepare high-value organolithiums,thereby significantly improving the economic profitability of LIB recycling.Organolithiums(R-O-Li and R-Li)were prepared using alkyl alcohol(R-OH)and alkyl bromide(R-Br)as substrates,where R includes varying hindered alkyl hydrocarbons.The organolithiums extracted from per kilogram of recycled LIBs can increase the economic value between$29.5 and$226.5 kg^(−1) cell.The value of the organolithiums is at least 5.4 times the total theoretical value of spent materials,improving the profitability of recycling LIBs over traditional pyrometallurgical($0.86 kg^(−1) cell),hydrometallurgical($1.00 kg^(−1) cell),and physical direct recycling methods($5.40 kg^(−1) cell).

关键词： lithiated graphite lithium-ion batteries recycling regeneration spent lithium-ion batteries

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