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Additives strategies to improving cycling stability of li metal batteries by modifying electrode electrolyte interphases

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Progress in Natural Science:Materials International 2024年第2期34卷 338-344页

作者： Yuan li Pengfei Huang Chunyu Cui Xiaoyuan Ma li Chen Zekun li linhai li Yuhong Tian School of Biological and Chemical Engineering Guangxi University of Science and Technology School of College of Chemistry and Chemical Engineering Hunan University Isky Future Energy Institute

li metal batteries（LMBs） have attracted much attention due to the ultra-high theoretical capacity of the li metal anode（LMA）.However,the uncontrollable dendrites growth and low coulombic efficiency hinder their practical ***,we explore 3,5-difluoropyridine（2F-BD） as a novel electrolyte additive to enable highperformance *** 2F-BD additive participates in and modifies the solvation structure of li ions by reducing the coordinated number of PF6-at the electrode surface,leading to the formation of a liF and li3N-rich solid electrolyte interphase（SEI）.The liF component increases the robustness of SEI and suppresses the formation of li dendrites,while the li3N component facilitates the transportation and reaction kinetics of li *** a result,the li‖li symmetric cell presents a stable cycling performance of up to 500 h at a current density of 1 mA *** coupling with liFePO4cathode,the obtained full cell achieves high specific capacities of 106.06 mA h g-1and 84.98 mA h g-1at 2.55 mA cm-2and 5.10 mA cm-2,respectively,and maintains a high capacity retention of84.0% after 1000 cycles at 0.13 mA cm-2,with an average cycling CE of 99.58%.

关键词： Electrolyte additive li dendrites li metal batteries liF and li3N-Rich electrode-electrolyte interphase liFePO4 cathode

Leaching kinetics of fluorine during the aluminum removal from spent li-ion battery cathode materials

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Journal of Environmental Sciences 2024年第4期138卷 312-325页

作者： Shengjie li Jianxin Zhu Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China

The high content of aluminum(Al)impurity in the recycled cathode powder seriously affects the extraction efficiency of Nickel,Cobalt,Manganese,and lithium resources and the actual commercial value of recycled materials,so Al removal is crucially important to conform to the industrial standard of spent li-ion battery cathode *** this work,we systematically investigated the leaching process and optimum conditions associated with Al removal from the cathode powder materials collected in a wet cathode-powder peeling and recycling production line of spent li-ion batteries(liBs).Moreover,we specifically studied the leaching of fluorine(F)synergistically happened along with the removal process of Al,which was not concerned about in other studies,but one of the key factors affecting pollution prevention in the recovery *** mechanism of the whole process including the leaching of Al and F from the cathode powder was indicated by using NMR,FTIR,and XPS,and a defluoridation process was preliminarily investigated in this *** leaching kinetics of Al could be successfully described by the shrinking core model,controlled by the diffusion process and the activation energy was 11.14 kJ/***,the leaching of F was attributed to the dissolution of liPF6and decomposition of PVDF,and the kinetics associated was described by Avrami *** interaction of Al and F is advantageous to realize the defluoridation to some *** is expected that our investigation will provide theoretical support for the large-scale recycling of spent liBs.

关键词： Al removal F leaching Cathode powder Heating alkali leaching Leaching kinetics

SEI/dead li-turning capacity loss for high-performance anode-free solid-state lithium batteries

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Journal of Energy Chemistry 2024年第9期96卷 145-152页

作者： Qianwen Yin Tianyu li Hongzhang Zhang Guiming Zhong Xiaofei Yang Xianfeng li Division of Energy Storage Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Key Laboratory of Long-Duration and Large-Scale Energy Storage Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Laboratory of Advanced Spectro-Electrochemistry and lithium-Ion Batteries Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal ***,the unclear mechanism for the fast capacity decay in AF-SSLBs,either determined by dead li or solid electrolyte interface(SEI),limits the proposal of effective strategies to prolong cycling *** clarify the underlying mechanism,herein,the evolution of SEI and dead li is quantitatively analyzed by a solid-state nuclear magnetic resonance(ss-NMR)technology in a typical liPF6-based polymer *** results show that the initial capacity loss is attributed to the formation of SEI,while the dead li dominates the following capacity loss and the growth rate is 0.141 mA h cm^(−2)cycle−*** reduce the active li loss,the combination of inorganic-rich SEI and self-healing electrostatic shield effect is proposed to improve the reversibility of li deposition/dissolution behavior,which reduces the capacity loss rate for the initial SEI and following dead li generation by 2.3 and 20.1 folds,*** a result,the initial Coulombic efficiency(ICE)and stable CE increase by 15.1%and 15.3%in li-Cu cells,which guides the rational design of high-performance AF-SSLBs.

关键词： Solid-state lithium batteries Solid-state NMR Anode-free SEI Dead li

Theoretical Design of Defects as a Driving Force for Ion Transport in li_(3)OBr Solid Electrolyte

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Energy & Environmental Materials 2024年第3期7卷 143-153页

作者： Xingyun Luo Yanlu li Xian Zhao State Key Lab of Crystal Materials and Institute of Crystal Materials Shandong UniversityJinan 250100China Center for Optics Research and Engineering Shandong UniversityQingdao 266237China

Due to ever-increasing concerns about safety issues in using li ionic batteries,solid electrolytes have extensively *** li-rich antiperovskite li_(3)OBr has been considered as a promising solid electrolyte candidate,but it still suffers challenges to achieve a high ionic conductivity owing to the high intrinsic symmetry of the crystal ***,we presented a design strategy that introduces various point defects and grain boundaries to break the high lattice symmetry of li_(3)OBr crystal,and their effect and microscopic mechanism of promoting the migration of li-ion were explored *** has been found that li_(i)are the dominant defects responsible for the fast li-ion diffusion in bulk li_(3)OBr and its surface,but they are easily trapped by the grain boundaries,leading to the annihilating of the Frenkel defect pair V'_(li)+li_(i),and thus limits the V'_(li)diffusion at the grain *** V_(Br)defect near the grain boundaries can effectively drive V'_(li)across the grain boundary,thereby converting the carrier of li^(+)migration from li,in the bulk and surface to V'_(li)at the grain boundary,and thus improving the ionic conductivity in the whole li_(3)OBr *** work provides a comprehensive insight into the li^(+)transport and conduction mechanism in the li_(3)OBr *** opens a new way of improving the conductivity for all-solid-state li electrolyte material through the defect design.

关键词： defects density functional theory ionic migration solid electrolyte

Highly polar CoP/Co_(2)P heterojunction composite as efficient cathode electrocatalyst for li-air battery

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Chinese Chemical Letters 2024年第9期35卷 486-490页

作者： Miaomiao li Mengwei Yuan Xingzi Zheng Kunyu Han Genban Sun Fujun li Huifeng li Beijing Key Laboratory of Energy Conversion and Storage Materials College of ChemistryBeijing Normal UniversityBeijing 100875China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Center for Advanced Materials Research Beijing Normal UniversityZhuhai 519087China

In order to advance the commercialization of rechargeable li-air batteries,it is of importance to explore cathode catalyst with efficient catalytic *** metal oxides have poor electrical conductivity,while cobalt phosphide has excellent electrical conductivity and large specific surface ***,its application in organic li-air batteries has been much less studied,and the electrocatalytic activity desires to be further ***,CoP/Co_(2)P heterojunction composite with higher polarity was *** discharge product of high-polarity CoP/Co_(2)P had a new porous box-like morphology,which was easy to be decomposed and exposed more active *** highly polar CoP/Co_(2)P heterostructure composite had homogeneous pores,the synergistic effect existed between CoP and Co_(2)P,and the discharge product was porous box mixed with li_(2)O_(2)and liOH,which made CoP/Co_(2)P achieve high specific capacity of14632 m Ah/g and cycle stably 161 times when used as air electrode cathode *** work furnished a thought for the construction of cathode catalysts with efficient catalytic activity for li-air batteries.

关键词： li-air battery Cathode catalyst CoP/Co_(2)P Heterojunction structure High polarity

Synergy effect of regulated li-plating and functional solid electrolyte interphase on graphite anodes

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Nano Research 2024年第9期17卷 8077-8085页

作者： Panpan Wang Baojia Xia Jianling li State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China Shanghai Institute of Microsystem and Information Technology Chinese Academy of SciencesShanghai 201800China

The growth of li dendrites poses potential safety hazard to lithium-ion batteries(liBs),and eliminating li dendrites thoroughly stills face tough difficulties ***,regulating li-plating is a critical optimization-direction to address the ***,a“graphite-li hybrid”anode with high reversibility is realized under the constant-capacity lithiation(CCL).Within CCL,the uniform distribution of li-plating on the graphite surface is successfully *** evolution in different states of solid electrolyte interphase(SEI)is investigated in detail to study the interaction between the potentials and impedance during the process of liintercalation and *** the potential below 0 V and the state of charge(SOC)of 110%relative to the theoretical capacity,the F-rich SEI with high stability is constructed to hinder the emergency of li dendrites and maintain the intact structure of graphite anode under long *** cell presents more than 100%Coulombic efficiency(CE)with the 900 cycles,demonstrating the reversible li-plating and the utilization of *** the CCL half-cell provides a good cycling performance and specific capacity of 900 cycles at 0.5 C,it is attributed to the synergy effect of stable inorganic-rich SEI and regulated active li-plating.

关键词： "graphite-li hybrid"anode li-plating reversibility solid electrolyte interphase(SEI)

Robust chemo-mechanical stability of additives-free SiO2anode realized by honeycomb nanolattice for high performance li-ion batteries

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Chinese Chemical Letters 2024年第10期35卷 468-472页

作者： Xinpin Pan Yongjian Cui Zhe Wang Bowen li Hailong Wang Jian Hao Feng li Jing li Advanced Energy Storage Materials Lab School of Materials and New Energy Ningxia University School of Chemistry and Chemical Engineering Ningxia University

Silicon-based anodes including Si, Si Oxand SiO2could deliver ultra-large capacities, but degrade fast owing to huge volume change and low conductivity. Generally, large amounts of elastic binder and conductive additives were composited with nanosized silicon-based materials to yield reasonable cycling stability, which nevertheless not only decrease specific capacity but also induce inhomogeneous lithiation/delithiation as well as uneven stress variations. Artificial nanolattice has exhibited superior mechanical properties which could be ideal structure for silicon-based anodes, but yet faces challenges in integration of chemical reactivity, conductivity and mechanical stability. Herein, we fabricate artificial SiO2honeycomb nanolattice consisting of numerous nanoscale SiO2cells interconnected by through-holes,and conformal coating of highly graphitic carbon on the nanolattice is achieved through in situ catalytic graphitization. Moreover, the nanolattice is firmly bonded on Cu substrate through atomic interdiffusion irrespective of surface roughness. This unique structure allows fast charge transportation and homogeneous lithiation/delithiation throughout the micron-meter nanolattice, which results in excellent stability and large reversible capacity over 500 cycles at 1 A/g. The results highlight design and constructing artificial nanolattice can be an effective way to prevent chemo-mechanical degradation of silicon-based anode materials.

关键词： Conductivity li-ion batteries Nanolattice SiO2 anode Stability

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小麦抗白粉病基因pm30种质改良及鉴定

华北农学报 2017年第A1期32卷 7-11页

作者：兰素缺李光威孟雅宁李芳张业伦李杏普河北省农林科学院粮油作物研究所河北省作物遗传育种实验室河北省现代农业产业技术体系小麦创新团队河北石家庄050035 河北省农林科学院经济作物研究所河北石家庄050051

白粉病是威胁我国乃至世界小麦生产的最主要病害之一。筛选和培育抗病品种是预防小麦感病减产的一条安全有效途径。为了将合成六倍体小麦中的白粉病抗病基因Pm30导入综合农艺性状好、产量高的优良小麦品种中,利用自育中抗白粉病的优良... 详细信息

白粉病是威胁我国乃至世界小麦生产的最主要病害之一。筛选和培育抗病品种是预防小麦感病减产的一条安全有效途径。为了将合成六倍体小麦中的白粉病抗病基因Pm30导入综合农艺性状好、产量高的优良小麦品种中,利用自育中抗白粉病的优良品系冀资356与合成小麦Synthetics(He-48)(*** PI94625/***)杂交,经过连续6年的选育,选育出高抗白粉病且农艺性状优良的品系7份。利用与Pm30连锁的SSR标记Xgwm159对这7份品系进行检测,用中国春和Pm30做对照,结果表明,14YF650和14YF675 2个品系扩增出430,460,500 bp条带,说明这2份材料携带来自于野生二粒小麦的抗白粉病基因Pm30。这2个品系表现矮秆抗倒、大穗、综合农艺性状较好,可以作为抗白粉病的亲本直接应用于抗病育种。

关键词：普通小麦野生二粒小麦抗病基因白粉病 Pm30 分子标记

Highly-chlorinated inert and robust interphase without mineralization of oxide enhancing high-rate li metal batteries

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Chinese Chemical Letters 2024年第6期35卷 239-243页

作者： Long li Kang Yang Chenpeng Xi Mengchao li Borong li Gui Xu Yuanbin Xiao Xiancai Cui Zhiliang liu lingyun li Yan Yu Chengkai Yang Key Laboratory of Advanced Materials Technologies International(HongKong Macao and Taiwan)Joint Laboratory on Advanced Materials TechnologiesSchool of Materials Science and EngineeringFuzhou UniversityFuzhou 350108China College of Material Sciences and Chemical Engineering Harbin Engineering UniversityHarbin 150001China

Side reactions and dendrite growth triggered by the unstable interface and inhomogeneous deposition have become the biggest obstacle to the commercialization for lithium metal *** this study,a highly-chlorinated organic-inorganic hybrid interfacial protective layer is developed by rationally tuning the interfacial passivation and robustness to achieve the convenient and efficient li metal *** polyvinyl chloride(PVC)can effectively resist water and oxygen,which is confirmed by density functional *** organic-dominant solid electrolyte interphases(SEI)with lithium chloride are investigated by the X-ray photoelectron spectroscopy(XPS)with little mineralization of oxide,such as li_(2)O and li_(2)CO_(3).With such artificial SEI,a uniform and dense lithium deposition morphology are formed and an ultra-long stable cycle of over 500 h are achieved even at an ultra-high current density of 10 m A/cm^(2).Moreover,the simple and convenient protected anode also exhibits excellent battery stability when paired with the liNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)and liFePO_(4)(LFP)cathode,showing great potential for the commercial application of lithium metal batteries.

关键词： Highly-chlorinated Water/oxygen resistance Stable interphase Dendrite-free lithium metal batteries High-rate