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lithium-Ion Charged Polymer Channels Flattening lithium Metal Anode

Nano-Micro Letters 2024年第4期16卷 379-393页

作者： Haofan Duan Yu You Gang Wang Xiangze Ou Jin Wen Qiao Huang Pengbo Lyu Yaru liang Qingyu li Jianyu Huang Yun‑Xiao Wang Hua‑Kun liu Shi Xue Dou Wei‑Hong Lai Hunan Provincial Key Laboratory of Thin Film Materials and Devices School of Material Sciences and EngineeringXiangtan UniversityXiangtan 411105People’s Republic of China Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemical and Pharmaceutical ScienceGuangxi Normal UniversityGuilin 541004People’s Republic of China Institute for Superconducting and Electronic Materials Australian Institute of Innovative MaterialsUniversity of WollongongInnovation CampusSquires WayNorth WollongongNSW 2500Australia Institute of Energy Materials Science University of Shanghai for Science and TechnologyShanghai 200093People’s Republic of China

The concentration difference in the near-surface region of lithium metal is the main cause of lithium dendrite growth.Resolving this issue will be key to achieving high-performance lithium metal batteries(LMBs).Herein,we construct a lithium nitrate(liNO_(3))-implanted electroactiveβphase polyvinylidene fluoride-co-hexafluoropropylene(PVDF-HFP)crystalline polymorph layer(PHL).The electronegatively charged polymer chains attain lithium ions on the surface to form lithium-ion charged channels.These channels act as reservoirs to sustainably release li ions to recompense the ionic flux of electrolytes,decreasing the growth of lithium dendrites.The stretched molecular channels can also accelerate the transport of li ions.The combined effects enable a high Coulombic efficiency of 97.0%for 250 cycles in lithium(li)||copper(Cu)cell and a stable symmetric plating/stripping behavior over 2000 h at 3 mA cm^(-2)with ultrahigh li utilization of 50%.Furthermore,the full cell coupled with PHL-Cu@li anode and li Fe PO_(4) cathode exhibits long-term cycle stability with high-capacity retention of 95.9%after 900 cycles.Impressively,the full cell paired with liNi_(0.87)Co_(0.1)Mn_(0.03)O_(2)maintains a discharge capacity of 170.0 mAh g^(-1)with a capacity retention of 84.3%after 100 cycles even under harsh condition of ultralow N/P ratio of 0.83.This facile strategy will widen the potential application of liNO_(3)in ester-based electrolyte for practical high-voltage LMBs.

关键词： Polymer ionic channel li metal batteries Artificial protective layer uniform li deposition Electrochemical performances

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A layered multifunctional framework based on polyacrylonitrile and MOF derivatives for stable lithium metal anode

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Journal of Energy Chemistry 2024年第6期93卷 282-288,I0007页

作者： Fanfan liu Peng Zuo Jing li Pengcheng Shi Yu Shao linwei Chen Yihong Tan Tao Ma Engineering Research Center of High-frequency Soft Magnetic Materials and Ceramic Powder Materials of Anhui Province School of Chemistry and Material EngineeringChaohu UniversityHefei 238024AnhuiChina Frontiers Science Center for Transformative Molecules School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China School of Pharmacy Anhui University of Chinese MedicineHefei 230012AnhuiChina School of Materials and Energy Guangdong University of TechnologyGuangzhou 510006GuangdongChina Jiujiang DeFu Technology Co. Ltd.Jiujiang 332000JiangxiChina

Composite li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable li metal batteries with high energy density.However,uneven li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of li ions.To promote uniform li deposition without top dendrite growth,herein,a layered multifunctional framework based on oxidation-treated polyacrylonitrile(OPAN) and metal-organic framework(MOF) derivatives was proposed for rationally regulating the distribution of li ions flux,nucleation sites,and electrical conductivity.Profiting from these merits,the OPAN/carbon nano fiber-MOF(CMOF) composite framework demonstrated a reversible li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm~2.Besides,such a li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells.When the li composite anode was paired with liFePO_(4)(LFP) cathode,the obtained full cell exhibited a stable cycling over 500 cycles.Moreover,the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design.These electrochemical and simulated results shed light on the difficulties of designing stable and safe li metal anode via optimizing the 3D frameworks.

关键词： lithium metal anode Layered multifunctional framework Ions flux redistribution Electrical insulation/conduction structure uniform li deposition

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Serrated lithium fluoride nanofibers-woven interlayer enables uniform lithium deposition for lithium-metal batteries

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National Science Review 2022年第11期9卷 194-207页

作者： Shuangshuang Tan Yalong Jiang Shuyan Ni Hao Wang Fangyu Xiong lianmeng Cui Xuelei Pan Chen Tang Yaoguang Rong Qinyou An liqiang Mai State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology College of Materials Science and Engineering Chongqing University Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory

The uncontrollable formation of li dendrites has become the biggest obstacle to the practical application of li-metal anodes in high-energy rechargeable li batteries. Herein, a unique liF interlayer woven by millimeter-level, single-crystal and serrated liF nanofibers(NFs) was designed to enable dendrite-free and highly efficient li-metal deposition. This high-conductivity li F interlayer can increase the li+transference number and induce the formation of ’li F–NFs-rich’ solid–electrolyte interface(SEI). In the ’li F–NFs-rich’SEI, the ultra-long li F nanofibers provide a continuously interfacial li+transport path. Moreover, the formed li–liF interface between li-metal and SEI film renders low li nucleation and high li+migration energy barriers, leading to uniform li plating and stripping processes. As a result, steady charge–discharge in a li//li symmetrical cell for 1600 h under 4 m Ah cm-2and 400 stable cycles under a high area capacity of 5.65 mAh cm-2in a high-loading li//rGO–S cell at 17.9 mA cm-2could be achieved. The free-standing liF –NFs interlayer exhibits superior advantages for commercial li batteries and displays significant potential for expanding the applications in solid li batteries.

关键词： lithium fluoride serrated nanofibers liF interlayer uniform li deposition lithium-metal batteries

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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 batteries.However,uncontrolled li dendrite growth during cycling remains a highly challenging drawback.To solve this problem,silver-coated graphene(Ag/GH)was prepared via a simple liquid-phase reduction method.The 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/GH.Ag was used as a lithiophilic nucleating agent to ensure uniform deposition of li and inhibit the growth of li dendrites on the anode.The prepared composite anode showed a significantly improved performance compared to the unmodified electrode.The 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 synthesis.Thus,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

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Multi-dimensional hybrid flexible films promote uniform lithium deposition and mitigate volume change as lithium metal anodes

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Journal of Energy Chemistry 2022年第2期31卷 583-591页

作者： Jian Yang Tingting Feng Junming Hou Xinran li Boyu Chen Cheng Chen Zhi Chen Yaochen Song Mengqiang Wu School of Materials and Energy University of Electronic Science and Technology of Chin1Chengdu 611731SichuanChina Yangtze Delta Region Institute(HuZhou) University of Electronic Science and Technology of Chin1Huzhou 313001ZhejiangChina

lithium metal is the ultimate anode material for next-generation high-energy batteries.Yet,the practical application of lithium metal anodes is limited by the formation of li dendrites and large volume changes.Herein,an effective multi-dimensional hybrid flexible film(MD-HFF)composed of iodine ion(0 dimension),CNTs(1 dimension)and graphene(2 dimensions)is designed for regulating li deposition and mitigating volume changes.The multi-dimensional components serve separate roles:(1)iodine ion enhances the conductivity of the electrode and provides lithiophilic sites,(2)CNTs strengthen interlaminar conductance and mechanical strength,acting as a spring in the layered structure to alleviate volume changes during li plating and stripping and(3)graphene provides mechanical flexibility and electrical conductivity.The resulting MD-HFF material supports stable li plating/stripping and high Coulombic efficiency(99%)over 230 cycles at 1 mA cm^(-2) with a deposition capacity of 1 mAh cm^(-2).Theoretical calculations indicate that liI contributes to the lateral growth of li on the MD-HFF surface,thereby inhibiting the formation of li dendrites.When paired with a typical NCM811 cathode,the assembled MD-HFF‖NCM811 cell exhibit improved capability and stable cycling performance.This research serves to guide material design in achieving li anode materials that do not suffer from dendrite formation and volume changes.

关键词： Flexible film li metal anode uniform li deposition Electrode volume change

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Stable lithium metal anode enabled by a robust artificial fluorinated hybrid interphase

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能源化学:英文版 2023年第8期83卷 612-621,I0014页

作者： Qiwen Ran Hongyuan Zhao Jintao liu Lei li Qiang Hu Jiangxuan Song Xingquan liu Sridhar Kormarneni School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 610054SichuanChina Departmentof Ecosystem Science and Management and Materials Research Institute 204 Energy and theEnvironment LaboratoryThePennsylvania State University University ParkPA 16802USA State Key Laboratory for Mechanical Behavior of Materials Shaanxi International Research Center for Soft MatterXi'an Jiaotong UniversityXi'an 710049ShaanxiChina Research Center for Electrochemistry and Energy Engineering Henan Institute of Science and TechnologyXinxiang 453003HenanChina

One of the key challenges for achieving stable lithium(li) metal anode is the construction of the rational solid electrolyte interphase(SEI),but its realization still faces enormous challenges.In this work,a robust artificial fluorinated hybrid interphase consisting of lithium-bismuth(li3Bi) alloy and lithium-fluoride(liF) was designed to regulate li deposition without li dendrite growth.The obtained hybrid interphase showed the high li+diffusion rate(3.5 × 10^(-4)S cm^(-1)),high electron resistivity(9.04 × 10^(4)Ω cm),and high mechanical strength(1348 MPa),thus enabling the uniform li deposition at the li/SEI interface.Specifically,li3Bi alloy,as a superionic conductor,accelerated the li+transport and stabilized the hybrid interphase.Meanwhile,liF was identified as a superior electron-blocker to inhibit the electron tunneling from the li anode into the SEI.As a result,the modified li anode showed the stable li plating/stripping behaviors over 1000 cycles even at 20 mA cm^(-2).Moreover,it also enabled the li(50 μm)‖liNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(4.4 mA h cm^(-2)) full cell to achieve an average Coulombic efficiency(CE) of 99.6%and a high-capacity retention of 79.2% after 100 cycles,whereas the bare li anode only exhibited a low-capacity retention of 8.0%.This work sheds light on the internal mechanism of li+transport within the hybrid interface and provides an effective approach to stabilize the interface of li metal anode.

关键词： li metal anode Artificial interphase li,Bi alloy liF uniform li deposition

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A 3D conducting scaffold with in-situ grown lithiophilic Ni_(2)P nanoarrays for high stability lithium metal anodes

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Journal of Energy Chemistry 2021年第3期30卷 301-309页

作者： Huai Jiang Hailin Fan Zexun Han Bo Hong Feixiang Wu Kai Zhang Zhian Zhang Jing Fang Yanqing Lai School of Metallurgy and Environment Central South UniversityChangsha 410083HunanChina Engineering Research Centre of Advanced Battery Materials The Ministry of EducationChangsha 410083HunanChina Contemporary Amperex Technology Co. Ltd.Ningde 352100FujianChina

lithium(li)metal is the most potential anode material for the next-generation high-energy rechargeable batteries.However,intrinsic surface unevenness and‘hostless’nature of li metal induces infinite volume effect and uncontrollable dendrite growth.Herein,we design the in-situ grown lithiophilic Ni_(2)P nanoarrays inside nickel foam(PNF).uniform Ni_(2)P nanoarrays coating presents a very low nucleation overpotential,which induces the homogeneous li deposition in the entire spaces of three-dimensional(3D)metal framework.Specifically,the lithiophilic Ni_(2)P nanoarrays possess characteristics of electrical conductivity and structural stability,which have almost no expansion and damage during repeating li plating/stripping.Therefore,they chronically inhibit the growth of li dendrites.This results in an outstanding Coulombic efficiency(CE)of 98% at 3 mA cm^(-2) and an ultra long cycling life over 2000 cycles with a low overpotential.Consequently,the PNF-li||liFePO_(4) battery maintains a capacity retention of 95.3% with a stable CE of 99.9% over 500 cycles at 2 C.

关键词： li metal anodes Ni_(2)P nanoarrays 3D metal framework uniform li deposition Superior lithiophilicity

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Boron-doping induced lithophilic transition of graphene for dendrite-free lithium growth

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Journal of Energy Chemistry 2021年第5期30卷 463-469页

作者： Wei liu Pengbo Zhai Shengjian Qin Jing Xiao Yi Wei Weiwei Yang Shiqiang Cui Qian Chen Chunqiao Jin Shubin Yang Yongji Gong School of Materials Science and Engineering Beihang UniversityBeijing 100191China School of Materials Science and Engineering Shijiazhuang Tiedao UniversityShijiazhuang 050043HebeiChina State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Electrochemical Process

li metal,possessing advantages of high theoretical specific capacity and low electrochemical potential,is regarded as the most promising anode material for next-generation batteries.However,despite decades of intensive research,its practical application is still hindered by safety hazard and low Coulombic efficiency,which is primarily caused by dendritic li deposition.To address this issue,restraining dendrite growth at the nucleation stage is deemed as the most effective method.By utilizing the difference of electronegativity between boron atoms and carbon atoms,carbon atoms around boron atoms in boron-doped graphene(BG)turn into lithiophilic sites,which can enhance the adsorption capacity to li^(+)at the nucleation stage.Consequently,an ultralow overpotential of 10 mV at a current density of 0.5 mA/cm^(2) and a high average Coulombic efficiency of 98.54%over more than 140 cycles with an areal capacity of 2 mAh/cm^(2) at a current density of 1 m A/cm^(2) were achieved.BG-li|liFePO_(4) full cells delivered a long lifespan of480 cycles at 0.5 C and excellent rate capability.This work provides a novel method for rational design of dendrite-free li metal batteries by regulating nucleation process.

关键词： lithium metal anode B-doped graphene lithophilic transition DFT calculation uniform li deposition

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Polybenzimidazole functionalized electrolyte with li-wetting and self-fluorination functionalities for practical li metal batteries

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InfoMat 2022年第5期4卷 174-186页

作者： Dongjiang Chen Yuanpeng liu Chuan Xia Yupei Han Qingwei Sun Xuchang Wang Wei Chen Xian Jian Weiqiang Lv Jianyi Ma Weidong He National Key Laboratory of Science and Technology on Advanced Composites in Special Environments and Center for Composite Materials and StructuresHarbin Institute of TechnologyHarbinChina School of Physics University of Electronic Science and Technology of ChinaChengduChina School of Materials and Energy University of Electronic Science and Technology of ChinaChengduChina Institute of Atomic and Molecular Physics Sichuan UniversityChengduSichuanChina

Rough li plating,low ionic conductivity,and low thermal stability of conventional electrolytes post-primary challenges for achieving reliable high-capacity rechargeable lithium batteries,for which lithiummetal is frequently proposed as themost promising anode material.Conventional low-polarity commercial polypropylene/polyethylene separators fail to support the application of high-energy-density li anodes due to their rigid physicochemical properties and the high reactivity of li metal,leading to fatal dendrite formation and vigorous exothermic reaction with electrolytes.Herein,we develop a li-wetting,flame-retardant binary polymer electrolyte by functionalizing poly(vinylidene fluoride)(PVDF)separators with nonflammable polybenzimidazole(PBI)to build safe room-temperature solid-state electrolyte membranes.A dendrite-free liFePO4 cell with the solid polymer electrolyte(SPE)delivers a discharge capacity of 127 mAh g^(-1) at 25℃ with a capacity retention of 87.5%after 500 cycles at 0.5℃(0.15 mA cm^(-2)).Phase-field simulations and density functional theory calculations demonstrate that the negatively charged benzimidazole chains of PBI own superior affinity to lithium bis(trifluoromethanesulfonyl)imide(liTFSI),and shares overlapping electron density with li anode,giving rise to accelerated li^(+)conduction at room temperature and uniform li electrodeposition at the electrolyte/li metal interface.The SPE is also flame-retardant since heat-resistant polytetrafluoroethylene and a dense,heat-blocking graphitized carbon layer are formed in intense heat throughdehydrogenation/fluorination of PVDF under the catalysis of Lewis base imidazole rings and the decomposition of benzimidazole rings in PBI.No such fire-resistant mechanism is ever reported in conventional electrolytes.

关键词： flame-retardant properties li metal polybenzimidazole solid polymer electrolyte uniform li deposition

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