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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

Improving li reversibility in li metal batteries through uniform dispersion of Ag nanoparticles on graphene

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Rare metals 2022年第10期41卷 3391-3400页

作者： Yu Gao Bing-Feng Cui Jia-Jun Wang Zhao-Yong Sun Qiang Chen Yi-Da Deng Xiao-Peng Han Wen-Bin Hu School of Materials Science and Engineering Tianjin Key Laboratory of Composite and Functional Materials Key Laboratory of Advanced Ceramics and Machining TechnologyTianjin UniversityTianjin300350China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou350207China China Energy lithium Co. LtdTianjin300072China State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou570228China

li metal is the most attractive and promising anode material for next-generation high-energy ***,uncontrolled li dendrite growth during cycling remains a highly challenging *** solve this problem,silver-coated graphene(Ag/GH)was prepared via a simple liquid-phase reduction *** effect of Ag/GH on li deposition behavior was investigated by adjusting the dispersion of Ag nanoparticles(Ag NPs).Subsequently,a composite electrode was fabricated via uniform deposition of metallic li on Ag/*** was used as a lithiophilic nucleating agent to ensure uniform deposition of li and inhibit the growth of li dendrites on the *** prepared composite anode showed a significantly improved performance compared to the unmodified *** symmetric cell comprising this composite electrode exhibited a stable cycling performance with a low hysteresis of~40 mV and a lifetime of>2000 h at a current density of 0.5 mA·cm^(-2).Meanwhile,the discharge capacity reached 0.5 mAh·cm^(-2).In addition,Ag/GH was found to be amenable to large-scale ***,the composite Ag/GH anode exhibited improved performance and the preparation method showed significant potential for application in the manufacture of li metal batteries.

关键词： Ag/graphene composite Uniform li deposition li anodes li metal batteries

MnO_(2) nanosheet modified N, P co-doping carbon nanofibers on carbon cloth as lithiophilic host to construct high-performance anodes for li metal batteries

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Journal of Energy Chemistry 2022年第6期31卷 270-281,I0008页

作者： Xiaoqiang liu Qian Zhang Yiru Ma Zhenzhen Chi Huixiang Yin Jie liu Junfei Huang Ziyang Guo Lei Wang Key Laboratory of Eco-chemical Engineering Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and TechnologyCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina College of Environment and Safety Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjin 300071China Key Laboratory of Eco-chemical Engineering Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and TechnologyCollege of Chemical EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina Shimadzu(China)Co. Ltd.Shenzhen BranchShenzhen 518000GuangdongChina

lithium (li) metal batteries have attracted much attention owing to its ultra-high energy ***,as important part of li metal batteries,li anodes still face many challenges,mainly including uncontrolled dendritic li formation,dramatical volume variation and serious ***,manganese dioxide (MnO_(2)) nanosheet modified nitrogen (N),phosphorus (P) co-doping carbon nanofibers(NPC) on carbon cloth (CC)(MnO_(2)@NPC-CC) is successfully fabricated through electrodeposition approach and further treated with li by the molten-infusion method to prepare li based Mn@NPC-CC(li-Mn@NPC-CC) *** synergy of MnO_(2) and NPC obviously increases the reaction rate between MnO_(2)@NPC-CC and li and guides even li distribution over infusion ***,theoretical calculation,simulation and experimental results further indicate that N,P,Mn multi-doping effectively improves the superior lithiophilicity of li-Mn@NPC-CC,which induces uniform li deposition/dissolution to suppress dendrite growth over ***,conductive and porous NPC matrix not only effectively improves the stability of li-Mn@NPC-CC,but also provides abundant spaces to accelerate the transfer of ion/electron and buffer electrode dimension variation during ***,li-Mn@NPC-CC-based symmetric cells exhibit extra-long cycling life (over 2200 h) with small hysteresis of 20 *** the liMn@NPC-CC anode couples with air,li iron phosphate (liFePO_(4)),or hard carbon (C) cathode,the assembled full cells exhibit outstanding performance with low hysteresis and stable cycling ***,the corresponding pouch-typed li–air cells also exhibit good performance at different bending angles and even power a series of electronic devices.

关键词： N,P co-doped carbon nanofibers on carbon cloth MnO_(2)nanosheet coating Molten-infusion method li metal anodes li metal batteries

Catalytic anode surface enabling in situ polymerization of gel polymer electrolyte for stable li metal batteries

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Nano Research 2024年第6期17卷 5216-5223页

作者： Guocheng li Kang liang Yuanjian li Xiangrui Duan lin Fu Zhao Cai Zhaofu Zhang Jiangnan Dai Yongming Sun Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China The Institute of Technological Sciences Wuhan UniversityWuhan 430074China Faculty of Materials Science and Chemistry China University of Geoscience(Wuhan)Wuhan 430074China

Employing quasi-solid-state gel polymer electrolyte(GPE)instead of the liquid counterpart has been regarded as a promising strategy for improving the electrochemical performance of li metal ***,the poor and uneven interfacial contact between li metal anode and GPE could cause large interfacial resistance and electrochemical li stripping/plating inhomogeneity,deteriorating the electrochemical ***,we proposed that the functional component of composite anode could work as the catalyst to promote the in situ polymerization reaction,and we experimentally realized the integration of polymerized-dioxolane electrolyte and li/li_(22)Sn_(5)/liF composite electrode with low interfacial resistance and good stability by in situ catalyzation ***,the reaction kinetics and stability of metallic li anode were significantly *** a demonstration,symmetric cell using such a GPE-li/li_(22)Sn_(5)/liF integration achieved stable cycling beyond 250 cycles with small potential hysteresis of 25 mV at 1 mA·cm^(−2)and 1 mAh·cm^(−2),far outperforming the counterpart regular GPE on pure *** with liNi0.5Co0.3Mn0.2O2,the full cell with the GPE-li/li_(22)Sn_(5)/liF integration maintained 85.7%of the original capacity after 100 cycles at 0.5 C(1 C=200 mA·g^(−1)).Our research provides a promising strategy for reducing the resistance between GPE and li metal anode,and realizes li metal batteries with enhance electrochemical performance.

关键词： catalyzation polymerization interface resistance interfacial stability li metal batteries electrochemical performance

Composite electrolyte with self-inserted structure and all-trans F conformation provides fast li^(+) transport for solid-state li metal batteries

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InfoMat 2024年第11期6卷 81-93页

作者： Ziyang liang Chang liu Xiang Bai Jiahui Zhang Xinyue Chang lixiang Guan Tiantian Lu Huayun Du Yinghui Wei Qian Wang Tao Wei Wen liu Henghui Zhou College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuanShanxithe People's Republic of China Shanxi Energy Internet Research Institute TaiyuanShanxithe People's Republic of China College of Chemistry and Molecular Engineering Peking UniversityBeijingthe People's Republic of China School of Energy and Power Jiangsu University of Science and TechnologyZhenjiangthe People's Republic of China State Key Lab of Chemical Resource Engineering College of Science and College of Energy Beijing University of Chemical TechnologyBeijingthe People's Republic of China

Solid-state li metal battery has attracted increasing interests for its potentiallyhigh energy density and excellent safety assurance, which is a promising candidatefor next generation battery system. However, the low ionic conductivityand li^(+) transport number of solid-state polymer electrolytes limit their practicalapplication. Herein, a composite polymer electrolyte with self-insertedstructure is proposed using the layered double hydroxides (LDHs) as dopant toachieve a fast li^(+) transport channel in poly(vinylidene-co-trifluoroethylene) [P(VDF-TrFE)] based polymer electrolyte. In such a composite electrolyte, P(VDF-TrFE) polymer has an all-trans conformation, in which all fluorineatoms locate on one side of the polymer chain, providing fast li^(+) transporthighways. Meanwhile, the LDH can immobilize the anions of li salts based onthe electrostatic interactions, promoting the dissociation of li salts, therebyenhancing the ionic conductivity (6.4 × 10^(-4) S cm^(-1)) and li^(+) transferencenumber (0.76). The anion immobilization effect can realize uniform electricfield distribution at the anode surface and suppress the dendritic li ***, the hydrogen bonding interaction between LDH and polymerchains also endows the composite electrolyte with strong mechanical ***, at room temperature, the li jj li symmetric cells can be stablycycled over 1000 h at a current density of 0.2 mA cm^(-2), and the full cells withliFePO_(4) cathode deliver a high capacity retention (>95%) after 200 cycles. This work offers a promising route to construct solid-state polymer electrolytes withfast li^(+) transport.

关键词： LDH li metal batteries li^(+) transport channel P(VDF-TrFE) solid-state polymer electrolytes

Diluent decomposition-assisted formation of li F-rich solid-electrolyte interfaces enables high-energy li-metal batteries

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Journal of Energy Chemistry 2023年第3期78卷 71-79,I0003页

作者： Junbo Zhang Haikuo Zhang Ruhong li ling Lv Di Lu Shuoqing Zhang Xuezhang Xiao Shujiang Geng Fuhui Wang Tao Deng lixin Chen Xiulin Fan Shenyang National Laboratory for Materials Science Northeastern UniversityShenyang 110819LiaoningChina State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Key Laboratory of Advanced Materials and Applications for batteries of Zhejiang Province Hangzhou 310013ZhejiangChina Department of Chemical and Biomolecular Engineering University of MarylandCollege Park 20742MDUSA

Passivation by the inorganic-rich solid electrolyte interphase(SEI),especially the liF-rich SEI,is highly desirable to guarantee the durable lifespan of li metal batteries(LMBs).Here,we report a diluent with the capability to facilitate the formation of liF-rich SEI while avoiding the excess consumption of li *** to most of reported inert diluents,heptafluoro-l-methoxypropane(HM) is firstly demonstrated to cooperate with the decomposition of anions to generate liF-rich SEI via releasing Fcontaining species near li *** designed electrolyte consisting of 1.8 M liFSI in the mixture of1,2-dimethoxyethane(DME)/HM(2:1 by vol.) achieves excellent compatibility with both li metal anodes(Coulombic efficiency~99.8%) and high-voltage cathodes(4.4 V liNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811) and 4.5 V liCoO_(2)(LCO) vs li^(+)/li).The 4.4 V li(20μm)‖NMC811(2.5 mA h cm^(-2)) and 4.5 V li(20μm)‖LCO(2.5 mA h cm^(-2)) cells achieve capacity retentions of 80% over 560 cycles and 80% over 505 cycles,***,the anode-free pouch cell delivers an energy density of~293 W h kg^(-1)initially and retains 70% of capacity after 100 deep *** work highlights the critical impact of diluent on the SEI formation,and opens up a new direction for designing desirable interfacial chemistries to enable high-performance LMBs.

关键词： Diluent Solvation structure liF-rich SEI li metal batteries Localized high-concentration electrolyte

A gradient solid electrolyte interphase with high li+conductivity induced by bisfluoroacetamide additive for stable lithium metal batteries

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Nano Research 2023年第6期16卷 8425-8432页

作者： Zhaoyang Sun Ziyue Wen Yi Chen Yue Ma Jinxiang Zhang Yuejiao li li li Renjie Chen Beijing Key Laboratory of Environmental Science and Engineering School of Material Science&EngineeringBeijing Institute of TechnologyBeijing 100081China Institute of Advanced Technology Beijing Institute of TechnologyJinan 250300China Collaborative Innovation Center of Electric Vehicles in Beijing Beijing 100081China

Stable li metal anodes have become the driving factor for high-energy-density battery ***,uncontrolled growth of li dendrite hinders the application of rechargeable li metal batteries(LMBs).Here,a multifunctional electrolyte additive bisfluoroacetamide(BFA)was proposed to facilitate high-performance *** uniform and dense deposition of li^(+) was achieved due to the reduced nucleation and plateau overpotential by the addition of ***,X-ray photoelectron spectroscopy(XPS)tests reveal a gradient solid electrolyte interface(SEI)structure on the li metal *** voltammetry(CV)curves at different sweep speeds prove the formation of pseudocapacitance at the electrode-electrolyte interface,which accelerates the li+transport rate and protects the electrode *** low activation energy also indicates the ability of rapid li^(+) transportation in electrolyte ***,the li||li symmetric cells with 1.0 wt.%BFA electrolyte exhibit good cycling performance at 0.5 mA·cm^(−2)for over 2000 h,and li||liNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)full cells maintain a high capacity for 200 cycles at 1 C rate.

关键词： electrolytes additives solid electrolyte interphase li dendrites li metal batteries

A robust Janus bilayer with tailored ionic conductivity and interface stability for stable li metal anodes

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Journal of Energy Chemistry 2022年第11期31卷 368-375,I0010页

作者： Guodong Zhang Pengwei li Kai Chen Hongfei Zheng Wei He liangping Xiao Xingyun li Qingchi Xu Jian Weng Jun Xu Department of Biomaterials College of MaterialsXiamen UniversityXiamen 361005FujianChina bDepartment of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional MaterialsXiamen UniversityXiamen 361005FujianChina Shenzhen Research Institute of Xiamen University Shenzhen 518057GuangdongChina

The formation and growth of li-dendrites caused by inhomogeneous li deposition severely hinder the commercial applications of li metal batteries due to the consequence of ***,we propose a Janus bilayer composed of black phosphorus(BP)and graphene oxide(GO)as an artificial interface with chemical/mechanical stability and well-regulated li-ion flux distribution for li metal anode *** to the synergy between the fast li-ion transport of BP in the inner layer and the high mechanical and chemical stability of GO in the outer layer,the GO/BP with good electrolyte wettability acts as a li-ion regulator that can induce homogeneous growth of li to suppress the li dendrites ***,long-term stability(500 h at 1 mA cm^(-2))with a low overpotential of 30 mV is achieved in the symmetric cell with GO/BP-li ***,the li–S cell with GO/BP-li exhibits enhanced cycling performance with a high capacity retention rate of 76.2%over 500 cycles at 1 C.

关键词： Graphene oxide(GO) Black phosphorus(BP) Artificial interface Janus bilayer li metal batteries

Unveiling the role of lithiophilic sites denseness in regulating lithium ion deposition

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Journal of Energy Chemistry 2022年第8期31卷 324-332,I0009页

作者： Tianlai Wu Yongyin Wang Weicai Zhang Kaixin Lu Jieyin Tan Mingtao Zheng Yong Xiao Yingliang liu Yeru liang Key Laboratory for Biobased Materials and Energy of Ministry of Education College of Materials and EnergySouth China Agricultural UniversityGuangzhou 510642GuangdongChina Guangdong Laboratory of lingnan Modern Agriculture Guangzhou 510642GuangdongChina

The construction of lithiophilic sites is an effective way to achieve uniform lithium(li)ion deposition for stably cycling li metal ***,in-depth investigations involving lithiophilic sites denseness(LSD)in impacting li ion deposition remain *** we propose an insight into this issue by probing the effect of LSD on determining the li ion *** characterization and theoretical simulation demonstrate that rational LSD plays a vital role in both li nucleation and the subsequent li ion plating *** tailoring the LSD from low to high,the accompanied li nucleation overpotentials continuously ***,the li ion mobility increases first and then weakens in the subsequent li ion plating ***,the li metal with a moderate LSD allows a dendritefree morphology and satisfactory long-term cycling *** work affords a deeper fundamental understanding of lithiophilic chemistry that directs the development of efficient strategies to realize dendrite-free li metal batteries.

关键词： li metal batteries lithiophilic sites denseness li nucleation li ion plating behaviour li dendrite inhibition

Deep eutectic solvent-based polymer electrolyte for solid-state lithium metal batteries

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Journal of Energy Chemistry 2022年第7期31卷 363-372,I0010页

作者： Panpan Dong Xiahui Zhang Kee Sung Han Younghwan Cha Min-Kyu Song School of Mechanical and Materials Engineering Washington State UniversityWA 99164United States Materials Sciences Pacific Northwest National LaboratoryWA 99352United States

Poly(ethylene) oxide(PEO)-based electrolytes have been widely studied for solid-state lithium batteries while their ionic conductivity and lithium-ion transference number still need to be further ***, using the combined experimental and theoretical approach, we demonstrate a novel, solidstate PEO-deep eutectic solvent(DES) electrolyte for the first time. We found that the in situ formation of DES can reduce the crystallinity of PEO matrix and more li+ions can move freely owing to the weakened coordination between ether oxygens and li-ions. Besides, we show that more li+ions can be dissociated from li salts in PEO-DES electrolyte using the molecular dynamics simulations. Such liquid-free PEO-DES electrolytes showed good ionic conductivity(2.1 × 10^(-4) S cm^(-1)) which is 160% higher than that of conventional PEO-li TFSI(8.1 × 10^(-5) S cm^(-1)) electrolyte at 60 ℃. Additionally, the PEO-DES electrolyte showed 136% increase of li-ion transference number(0.33) compared with ionic liquid-doped PEO-li TFSI(0.14) at 60 ℃. Moreover, the PEO-DES exhibited good compatibility with li metal and stable li plating/stripping behavior with little morphology change of li metal. This research also provides new insights into the enhancement mechanisms of novel polymer electrolytes, improving our fundamental understanding of critical challenges that have impeded the adoption of solid-state lithium metal batteries.

关键词： Deep eutectic solvent li metal batteries PEO Solid-state electrolytes li plating/stripping