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Viability of all-solid-state lithium metal battery coupled with oxide solid-state electrolyte and high-capacity cathode
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作者 Xingxing Jiao Xieyu Xu +6 位作者 Yongjing Wang Xuyang Wang Yaqi Chen Shizhao Xiong Weiqing Yang Zhongxiao Song Yangyang Liu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期122-131,共10页
Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g^(-1)and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La_(3)Zr_(2)O_(12)(LLZO),a... Owing to the utilization of lithium metal as anode with the ultrahigh theoretical capacity density of 3860 mA h g^(-1)and oxide-based ceramic solid-state electrolytes(SE),e.g.,garnet-type Li7La_(3)Zr_(2)O_(12)(LLZO),all-state-state lithium metal batteries(ASLMBs)have been widely accepted as the promising alternatives for providing the satisfactory energy density and safety.However,its applications are still challenged by plenty of technical and scientific issues.In this contribution,the co-sintering temperature at 500℃is proved as a compromise method to fabricate the composite cathode with structural integrity and declined capacity fading of LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2)(NCM).On the other hand,it tends to form weaker grain boundary(GB)inside polycrystalline LLZO at inadequate sintering temperature for LLZO,which can induce the intergranular failure of SE during the growth of Li filament inside the unavoidable defect on the interface of SE.Therefore,increasing the strength of GB,refining the grain to 0.4μm,and precluding the interfacial defect are suggested to postpone the electro-chemo-mechanical failure of SE with weak GB.Moreover,the advanced sintering techniques to lower the co-sintering temperature for both NCM-LLZO composite cathode and LLZO SE can be posted out to realize the viability of state-of-the-art ASLMBs with higher energy density as well as the guaranteed safety. 展开更多
关键词 All-solid-state lithium metal battery LiNi_(0.5C)o_(0.2)Mn_(0.3)O_(2)-Li7La_(3)Zr_(2)O_(12)composite cathode CO-SINTERING lithium metal anode Electro-chemo-mechanical failure
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Modification of Li Anode with Perfluorodecyltrimethoxysilane to Enhance the Performance of Lithium Metal Battery
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作者 Yinghan Shao 《Journal of Power and Energy Engineering》 2024年第8期70-77,共8页
The solid electrolyte interphase (SEI) on the surface of lithium metal anodes can dictate the electrochemical performance of lithium-metal-based batteries. Due to ineffective adhesion, the natural SEI layer may detach... The solid electrolyte interphase (SEI) on the surface of lithium metal anodes can dictate the electrochemical performance of lithium-metal-based batteries. Due to ineffective adhesion, the natural SEI layer may detach from the lithium negative electrode during interface fluctuations, thereby deteriorating the electrochemical performance of lithium-metal-based batteries. This work introduces perfluorosiloxane coupling agents as interfacial adhesion promoters, chemically bonding and physically entangling the lithium metal with the SEI via the formation of Li-O-Si bonds with the inorganic reactive groups anchoring to the Li substrate and the organic functional groups participating in the formation of the SEI layer, thus binding with its components. Lithium metal batteries modified with silane coupling agents exhibit superior electrochemical performance compared to unmodified lithium metal batteries. The modified lithium metal battery retains a specific capacity of 162 mAh/g after 200 cycles, while the unmodified lithium metal battery only retains 140 mAh/g. 展开更多
关键词 lithium metal battery SEI High Density PFDTMS Surface
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A fast ionic transport copolymeric network for stable quasi-solid lithium metal battery 被引量:2
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作者 Weiqi Mai Qiaoying Cao +4 位作者 Mingtao Zheng Yong Xiao Hang Hu Yingliang Liu Yeru Liang 《Journal of Energy Chemistry》 SCIE EI CSCD 2023年第12期491-500,I0013,共11页
Solid-state lithium(Li) metal batteries overwhelm the lithium-ion batteries by harvesting high energy from Li metal anode with ultrahigh capacities and gaining excellent safety from solid electrolytes.However,the unco... Solid-state lithium(Li) metal batteries overwhelm the lithium-ion batteries by harvesting high energy from Li metal anode with ultrahigh capacities and gaining excellent safety from solid electrolytes.However,the uncontrollable solvents in solid electrolytes usually aggravate poor interfacial contact with lithium metal anode and deteriorate Li^(+) pathways.Here a copolymeric network-structured ion conductor by rationally integrating cellulose nanofibril as a two-in-one functional material is employed to anchor the solvent.Taking advantages of tightly anchoring of cellulose nanofibril to solvent,the asconstructed quasi-solid polymer-based electrolyte offers rapid Li^(+) transport channels and realizes effective Li-dendrite suppression,which enables high ionic conductivity of 1.93 × 10^(-3)S cm^(-1) at room temperature,long-term Li plating/stripping over 1900 h,and high capacity retention of 99%.This work provides a fresh strategy for creating solid electrolytes that meet both high ionic conductivity and interfacial stability requirements for practical solid-state lithium metal battery. 展开更多
关键词 lithium metal battery Quasi-solid polymer electrolyte Cellulose nanofibrils Solvent anchoring Copolymeric network
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Dependence of lithium metal battery performances on inherent separator porous structure regulation
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作者 Lei Ding Dandan Li +7 位作者 Lingyang Liu Pengfang Zhang Fanghui Du Chao Wang Daoxin Zhang Shuo Zhang Sihang Zhang Feng Yang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第9期436-447,共12页
Boosting of rechargeable lithium metal batteries(LMBs) holds challenges because of lithium dendrites germination and high-reactive surface feature.Separators may experience structure-determined chemical deterioration ... Boosting of rechargeable lithium metal batteries(LMBs) holds challenges because of lithium dendrites germination and high-reactive surface feature.Separators may experience structure-determined chemical deterioration and worsen Li plating-stripping behaviors when smoothly shifting from lithium-ion batteries(LIBs) to LMBs.This study precisely regulations the crystal structure of β-polypropylene and separator porous construction to investigate the intrinsic porous structure and mechanical properties determined electrochemical performances and cycling durability of LMBs.Crystal structure characterizations,porous structure analyses,and electrochemical cycling tests uncover appropriate annealing thermal stimulation concentrates β-lamellae thickness and enhances lamellae thermal stability by rearranging molecular chain in inferior β-lamellae,maximally homogenizing biaxial tensile deformation and resultant porous constructions.These even pores with high connectivity lower ion migration barriers,alleviate heterogeneous Li^(+) flux dispersion,stabilize reversible Li plating-stripping behaviors,and hinder coursing and branching of Li dendrites,endowing steady cell cycling durability,especially at higher currents due to the highlighted uncontrollable cumulation of dead Li,which offers new insights for the current pursuit of high-power density battery and fast charging technology.The suggested separator structure-chemical nature functions in ensuring cyclic cell stability and builds reliable relationships between separator structure design and practical LMBs applications. 展开更多
关键词 lithium metal battery Polyolefin separator Porous structure design lithium dendrite regulation Cycling stability
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High-performance all-solid-state polymer electrolyte with fast conductivity pathway formed by hierarchical structure polyamide 6 nanofiber for lithium metal battery 被引量:5
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作者 Lu Gao Jianxin Li +3 位作者 Jingge Ju Bowen Cheng Weimin Kang Nanping Deng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第3期644-654,共11页
The utilization of all-solid-state electrolytes is considered to be an effective way to enhance the safety performance of lithium metal batteries.However,the low ionic conductivity and poor interface compatibility gre... The utilization of all-solid-state electrolytes is considered to be an effective way to enhance the safety performance of lithium metal batteries.However,the low ionic conductivity and poor interface compatibility greatly restrict the development of all-solid-state battery.In this study,a composite electrolyte combining the electrospun polyamide 6(PA6)nanofiber membrane with hierarchical structure and the polyethylene oxide(PEO)polymer is investigated.The introduction of PA6 nanofiber membrane can effectively reduce the crystallinity of the polymer,so that the ionic conductivity of the electrolyte can be enhanced.Moreover,it is found that the presence of finely branched fibers in the hierarchical structure PA6 membrane allows the polar functional groups(C=O and N-H bonds)to be fully exposed,which provides sufficient functional sites for lithium ion transport and helps to regulate the uniform deposition of lithium metal.Moreover,the hierarchical structure can enhance the mechanical strength(9.2 MPa)of the electrolyte,thereby effectively improving the safety and cycle stability of the battery.The prepared Li/Li symmetric battery can be stably cycled for 1500 h under 0.3 mA cm^(-2) and 60℃.This study demonstrates that the prepared electrolyte has excellent application prospects in the next generation all-solid-state lithium metal batteries. 展开更多
关键词 Hierarchical structure PA6 electrospun nanofiber membrane All-solid-state composite polymer electrolyte lithium metal battery
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Dendrite‑Free and Stable Lithium Metal Battery Achieved by a Model of Stepwise Lithium Deposition and Stripping 被引量:3
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作者 Tiancun Liu Jinlong Wang +2 位作者 Yi Xu Yifan Zhang Yong Wang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2021年第11期155-167,共13页
The uncontrolled formation of lithium(Li)dendrites and the unnecessary consumption of electrolyte during the Li plating/stripping process have been major obstacles in developing safe and stable Li metal batteries.Here... The uncontrolled formation of lithium(Li)dendrites and the unnecessary consumption of electrolyte during the Li plating/stripping process have been major obstacles in developing safe and stable Li metal batteries.Herein,we report a cucumber-like lithiophilic composite skeleton(CLCS)fabricated through a facile oxidationimmersion-reduction method.The stepwise Li deposition and stripping,determined using in situ Raman spectra during the galvanostatic Li charging/discharging process,promote the formation of a dendrite-free Li metal anode.Furthermore,numerous pyridinic N,pyrrolic N,and CuxN sites with excellent lithiophilicity work synergistically to distribute Li ions and suppress the formation of Li dendrites.Owing to these advantages,cells based on CLCS exhibit a high Coulombic efficiency of 97.3%for 700 cycles and an improved lifespan of 2000 h for symmetric cells.The full cells assembled with LiFePO_(4)(LFP),SeS_(2) cathodes and CLCS@Li anodes demonstrate high capacities of 110.1 mAh g^(−1) after 600 cycles at 0.2 A g^(−1) in CLCS@Li|LFP and 491.8 mAh g^(−1) after 500 cycles at 1 A g^(−1) in CLCS@Li|SeS2.The unique design of CLCS may accelerate the application of Li metal anodes in commercial Li metal batteries. 展开更多
关键词 Lithiophilic skeleton Stepwise Li deposition and stripping Dendrite suppression lithium metal battery Electrochemical properties
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Block copolymer electrolyte with adjustable functional units for solid polymer lithium metal battery 被引量:2
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作者 Zhiyuan Lin Xianwei Guo +3 位作者 Yubo Yang Mingxue Tang Qi Wei Haijun Yu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第1期67-74,I0003,共9页
Solid polymer electrolytes have been considered as the promising candidates to improve the safety and stability of high-energy lithium metal batteries.However,the practical applications of solid polymer electrolytes a... Solid polymer electrolytes have been considered as the promising candidates to improve the safety and stability of high-energy lithium metal batteries.However,the practical applications of solid polymer electrolytes are still limited by the low ionic conductivity,poor interfacial contact with electrodes,narrow electrochemical window and weak mechanical strength.Here,a series of novel block copolymer electrolytes with three-dimensional networks are designed by cross-linked copolymerization of the polyethylene glycol soft segments and hexamethylene diisocyanate trimer hard segments.Their ionic migration performances and interface compatibilities with Li metal anode have been optimized delicately by tailoring the ratio of these functional units.The optimized block copolymer electrolyte has shown an amorphous crystalline structure,a high ionic conductivity of ~5.7×10^(-4)S cm^(-1),high lithium ion transference number(~0.49),wide electrochemical window up to ~4.65 V(vs.Li+/Li) and favorable mechanical strength at 55℃.Furthermore,the enhanced interface compatibility can well support the normal operations of lithium metal batteries using both LiFePO4 and LiNi0.8Co0.15Al0.05O2 cathodes.This study not only paves a new way to develop solid polymer electrolyte with optimizing functional units,but also provides a polymer electrolyte design strategy for the application demand of lithium metal battery. 展开更多
关键词 Block copolymer electrolyte Functional units Ionic migration performance Interface compatibility lithium metal battery
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A lithiated gel polymer electrolyte with superior interfacial performance for safe and long-life lithium metal battery 被引量:1
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作者 Jia-Jia Yuan Chuang-Chao Sun +6 位作者 Li-Feng Fang You-Zhi Song Yan Yan Ze-Lin Qiu Yu-Jie Shen Han-Ying Li Bao-Ku Zhu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第4期313-322,共10页
Rechargeable lithium metal batteries(LMBs)have gained much attention recently.However,the short lifespan and safety issues restrict their commercial applications.Here we report a novel gel polymer electrolyte(GPE)base... Rechargeable lithium metal batteries(LMBs)have gained much attention recently.However,the short lifespan and safety issues restrict their commercial applications.Here we report a novel gel polymer electrolyte(GPE)based on lithiated poly(vinyl chloride-r-acrylic acid)(PVCAALi)to realize dendritesuppressing and long-term stable lithium metal cycling.PVC chains ensure the quick gelation process and high electrolyte uptake,and lithiated PAA segments enable the increase of mechanical strength,acceleration of lithium-ion transmission and improvement of interfacial compatibility.PVCAALi GPE showed much higher mechanical strength compared with other free-standing GPEs in previous works.It displays a superior ionic conductivity of 1.50 m S cm^(-1) and a high lithium-ion transference number of 0.59 at room temperature.Besides,the lithiated GPE exhibits excellent interfacial compatibility with lithium metal anodes.Lithium symmetrical cells with PVCAALi GPE yield low hysteresis of 50 m V over1000 h at 1.0 m A cm^(-2).And the possible mechanism of the lithiated GPE with improved lithium-ion transfer and interfacial property was discussed.Accordingly,both the Li4Ti5O12/Li and lithium-sulfur(Li-S)cells assembled with PVCAALi GPE show outstanding electrochemical performance,retaining high discharge capacities of 133.8 m Ah g^(-1) and 603.8 m Ah g^(-1) over 200 cycles,respectively.This work proves excellent application potential of the highly effective and low-cost PVCAALi GPE in safe and long-life LMBs. 展开更多
关键词 LITHIATION Gel polymer electrolyte lithium dendrite Safety lithium metal battery
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Enhanced electrochemical performance of garnet-based solid-state lithium metal battery with modified anodic and cathodic interfaces
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作者 Deen Yan Huangwang Mai +3 位作者 Wen Chen Wei Yang Hanbo Zou Shengzhou Chen 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第4期140-147,共8页
Due to high ionic conductivity and wide electrochemical window,the garnet solid electrolyte is considered as the most promising candidate electrolyte for solid-state lithium metal batteries.However,the high contact im... Due to high ionic conductivity and wide electrochemical window,the garnet solid electrolyte is considered as the most promising candidate electrolyte for solid-state lithium metal batteries.However,the high contact impedance between metallic lithium and the garnet solid electrolyte surface seriously hampers its further application.In this work,a Li-(ZnO)_(x)anode is prepared by the reaction of zinc oxide with metallic lithium and in situ coated on the surface of Li_(6.8)La_(3)Zr_(1.8)Ta_(0.2)O_(12)(LLZTO).The anode can be perfectly bound to the surface of LLZTO solid electrolyte,and the anode/electrolyte interfacial resistance was reduced from 2319 to 33.75Ω·cm^(2).The Li-(ZnO)_(0.15)|LLZTO|Li-(ZnO)_(0.15) symmetric battery exhibits a stable Li striping/plating process during charge-discharging at a constant current density of0.1 m A·cm;for 100 h at room temperature.Moreover,a Li-(ZnO)_(0.15)|LLZTO-SPE|LFP full battery,comprised of a polyethylene oxide-based solid polymer electrolyte(SPE)film as an interlayer between LiFePO4(LFP)cathode and LLZTO solid electrolyte,presents an excellent performance at 60℃.The discharge capacity of the full battery reaches 140 mA·h·g^(-1)at 0.1 C and the capacity attenuation is less than3%after 50 cycles. 展开更多
关键词 lithium metal battery Solid-state electrolyte Li-ZnO anode
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Metal-organic nanosheet assembly ions sieving membrane for precise lithium ion and anion/solvent separation toward robust lithium metal battery
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作者 Jian-Qiang Shen Tian-Tian Zhao +5 位作者 Ying-Li Song Lingjuan Zhang Ya-Nan Gao Xiao-Nan Cui Peng Zhao Xian-Ming Zhang 《Science China Chemistry》 SCIE EI CAS CSCD 2024年第10期3320-3327,共8页
Metal-organic nanosheets(MONs)as a novel material with tunable pore structures and low mass transfer resistance,have emerged as molecular sieves for the separation of gases and liquids.In theory,they can also serve as... Metal-organic nanosheets(MONs)as a novel material with tunable pore structures and low mass transfer resistance,have emerged as molecular sieves for the separation of gases and liquids.In theory,they can also serve as ion sieves for lithium metal batteries(LMBs),realizing the high-energy and dendritic free LMBs.However,there are rarely relevant reports,because it is difficult to simultaneously balance efficient ion sieving ability,high ion passing rate and high electrochemical stability.Here,we synthesized a stable ultrathin MON[Zn_(2)(Bim)_(4)]([Zn_(2)(Bim)_(4)]Nanosheet,HBim=benzimidazolate),which can achieve both efficient lithium ion sieving ability,high lithium ion passing rate and high electrochemical stability at the same time.The separator assembled by this MON exhibits high Li^(+)transfer number of 0.81 due to the accurate lithium ion and anion/solvent separation.The battery containing such separator shows high lithium ionic conductivity of 0.74 m S cm^(-1)and low activation energy of 0.099 eV,which can be attributed to the nanometer level thickness and the ion sieving effect.What is more,we realized the application of MONs-based ion sieves in LMBs with intercalation cathodes for the first time.And the LiFePO_(4)|Li battery with as-assembled separator demonstrates improved Coulombic efficiency(>99%)and significantly extended cycling life(>1600 cycles)with 80%capacity retention. 展开更多
关键词 lithium sieving membrane metal-organic nanosheets lithium metal battery lithium ion and anion separation lithium ion and solvent separation
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Formatted PVDF in lamellar composite solid electrolyte for solidstate lithium metal battery
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作者 Xinji Zhang Yafang Zhang +4 位作者 Shiyue Zhou Jingchuan Dang Chenye Wang Wenjia Wu Jingtao Wang 《Nano Research》 SCIE EI CSCD 2024年第6期5159-5167,共9页
Solid polymer electrolytes(SPEs)hold great application potential for solid-state lithium metal battery because of the excellent interfacial contact and processibility,but being hampered by the poor room-temperature co... Solid polymer electrolytes(SPEs)hold great application potential for solid-state lithium metal battery because of the excellent interfacial contact and processibility,but being hampered by the poor room-temperature conductivity(~10^(−7)S·cm^(−1))and low lithium-ion transference number(tLi+).Here,a lamellar composite solid electrolyte(Vr-NH_(2)@polyvinylidene fluoride(PVDF)LCSE)withβ-conformation PVDF is fabricated by confining PVDF in the interlayer channel of-NH_(2)modified vermiculite lamellar framework.We demonstrate that the conformation of PVDF can be manipulated by the nanoconfinement effect and the interaction from channel wall.The presence of-NH_(2)groups could induce the formation ofβ-conformation PVDF through electrostatic interaction,which serves as continuous and rapid lithium-ion transfer pathway.As a result,a high room-temperature ionic conductivity of 1.77×10^(−4)S·cm^(−1)is achieved,1-2 orders of magnitude higher than most SPEs.Furthermore,Vr-NH_(2)@PVDF LCSE shows a high tLi+of 0.68 because of the high dielectric constant,~3 times of that of PVDF SPE,and surpassing most of reported SPEs.The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)||Li cell assembled by Vr-NH_(2)@PVDF LCSE obtains a discharge specific capacity of 137.1 mAh·g^(−1)after 150 cycles with a capacity retention rate of 93%at 1 C and 25℃.This study may pave a new avenue for high-performance SPEs. 展开更多
关键词 solid-state lithium metal battery lamellar composite solid electrolyte β-conformation polyvinylidene fluoride(PVDF) room-temperature ionic conductivity lithium-ion transference number
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3D core-shell nanofibers framework and functional ceramic nanoparticles synergistically reinforced composite polymer electrolytes for high-performance all-solid-state lithium metal battery
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作者 Hengying Xiang Nanping Deng +3 位作者 Lu Gao Wen Yu Bowen Cheng Weimin Kang 《Chinese Chemical Letters》 SCIE CAS CSCD 2024年第8期425-432,共8页
Satisfactory ionic conductivity,excellent mechanical stability,and high-temperature resistance are the prerequisites for the safe application of solid polymer electrolytes(SPEs)in all-solid-state lithium metal batteri... Satisfactory ionic conductivity,excellent mechanical stability,and high-temperature resistance are the prerequisites for the safe application of solid polymer electrolytes(SPEs)in all-solid-state lithium metal batteries(ASSLMBs).In this study,a novel poly(m-phenylene isophthalamide)(PMIA)-core/poly(ethylene oxide)(PEO)-shell nanofiber membrane and the functional Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)ceramic nanopar-ticle are simultaneously introduced into the PEO-based SPEs to prepare composite polymer electrolytes(CPEs).The core PMIA layer of composite nanofibers can greatly improve the mechanical strength and thermal stability of the CPEs,while the shell PEO layer can provide the 3D continuous transport channels for lithium ions.In addition,the introduction of functional LLZTO nanoparticle not only reduces the crys-tallinity of PEO,but also promotes the dissociation of lithium salts and releases more Li^(+)ions through its interaction with the Lewis acid-base of anions,thereby overall improving the transport of lithium ions.Consequently,the optimized CPEs present high ionic conductivity of 1.38×10^(−4)S/cm at 30℃,signifi-cantly improved mechanical strength(8.5 MPa),remarkable thermal stability(without obvious shrinkage at 150℃),and conspicuous Li dendrites blocking ability(>1800 h).The CPEs also both have good com-patibility and cyclic stability with LiFePO_(4)(>2000 cycles)and high-voltage LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2)(NMC811)(>500 cycles)cathodes.In addition,even at low temperature(40℃),the assembled LiFePO4/CPEs/Li bat-tery still can cycle stably.The novel design can provide an effective way to exploit high-performance solid-state electrolytes. 展开更多
关键词 Composite polymer electrolytes Core-shell structured nanofiber Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)ceramic nanoparticle All-solid-state lithium metal batteries Outstanding thermal stability and electrochemical performance
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From Liquid to Solid‑State Lithium Metal Batteries:Fundamental Issues and Recent Developments
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作者 Zhao Zhang Wei‑Qiang Han 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第2期68-125,共58页
The widespread adoption of lithium-ion batteries has been driven by the proliferation of portable electronic devices and electric vehicles,which have increasingly stringent energy density requirements.Lithium metal ba... The widespread adoption of lithium-ion batteries has been driven by the proliferation of portable electronic devices and electric vehicles,which have increasingly stringent energy density requirements.Lithium metal batteries(LMBs),with their ultralow reduction potential and high theoretical capacity,are widely regarded as the most promising technical pathway for achieving high energy density batteries.In this review,we provide a comprehensive overview of fundamental issues related to high reactivity and migrated interfaces in LMBs.Furthermore,we propose improved strategies involving interface engineering,3D current collector design,electrolyte optimization,separator modification,application of alloyed anodes,and external field regulation to address these challenges.The utilization of solid-state electrolytes can significantly enhance the safety of LMBs and represents the only viable approach for advancing them.This review also encompasses the variation in fundamental issues and design strategies for the transition from liquid to solid electrolytes.Particularly noteworthy is that the introduction of SSEs will exacerbate differences in electrochemical and mechanical properties at the interface,leading to increased interface inhomogeneity—a critical factor contributing to failure in all-solidstate lithium metal batteries.Based on recent research works,this perspective highlights the current status of research on developing high-performance LMBs. 展开更多
关键词 lithium metal batteries All-solid-state lithium metal battery Li dendrite Solid electrolyte Interface
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Converting an O-vacancy-rich oxide into a multifunctional separator modifier for long-lifespan lithium metal batteries
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作者 Juntao Si Xiaoying Li +3 位作者 Yixuan Li Kuo Cao Yiran Zhu Chunhua Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第10期371-378,I0007,共9页
The lithium metal anode is hailed as the desired "holy grail" for the forthcoming generation of highenergy-density batteries,given its astounding theoretical capacity and low potential.Nonetheless,the format... The lithium metal anode is hailed as the desired "holy grail" for the forthcoming generation of highenergy-density batteries,given its astounding theoretical capacity and low potential.Nonetheless,the formation and growth of dendrites seriously compromise battery life and safety.Herein,an yttriastabilized bismuth oxide(YSB) layer is fabricated on the polypropylene(PP) separator,where YSB reacts with Li anode in-situ in the cell to form a multi-component composite interlayer consisting of Li_(3)Bi,Li_(2)O,and Y_(2)O_(3).The interlayer can function not only as a redistributor to regulate Li^(+) distribution but also as an anion adsorber to increase the Li^(+) transference number from 0.37 to 0.79 for suppressing dendrite nucleation and growth.Consequently,compared with the cell with a baseline separator,those with modified separators exhibit prolonged lifespan in both Li/Li symmetrical cells and Li/Cu half-cells.Notably,the full cells coupled with ultrahigh-loading LiFePO_(4) display an excellent cycling performance of 1700 cycles with a high capacity retention of ~80% at 1 C,exhibiting great potential for practical applications.This work provides a feasible and effective new strategy for separator modification towards building a much-anticipated dendrite-free Li anode and realizing long-lifespan lithium metal batteries. 展开更多
关键词 lithium metal battery SEPARATOR Dendrite-free Multifunctional interlayer Conversion-alloying reaction
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Postmortem ^(7)Li NMR analysis for assessing the reversibility of lithium metal electrodes in lithium metal batteries
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作者 Jaewon Baek Sunha Kim +1 位作者 Hee-Tak Kim Oc Hee Han 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第7期430-440,共11页
Despite the proficiency of lithium(Li)-7 NMR spectroscopy in delineating the physical and chemical states of Li metal electrodes,challenges in specimen preparation and interpretation impede its progress.In this study,... Despite the proficiency of lithium(Li)-7 NMR spectroscopy in delineating the physical and chemical states of Li metal electrodes,challenges in specimen preparation and interpretation impede its progress.In this study,we conducted a comprehensive postmortem analysis utilizing ^(7)Li NMR,employing a stan-dard magic angle spinning probe to examine protective-layer coated Li metal electrodes and LiAg alloy electrodes against bare Li metal electrodes within Li metal batteries(LMBs).Our investigation explores the effects of sample burrs,alignment with the magnetic field,the existence of liquid electrolytes,and precycling on the ^(7)Li NMR signals.Through contrasting NMR spectra before and after cycling,we identi-fied alterations in Li^(0) and Li^(+) signals attributable to the degradation of the Li metal electrode.Our NMR analyses decisively demonstrate the efficacy of the protective layer in mitigating dendrite and solid elec-trolyte interphase formation.Moreover,we noted that Li*ions near the Li metal surface exhibit magnetic susceptibility anisotropy,revealing a novel approach to studying diamagnetic species on Li metal elec-trodes in LMBs.This study provides valuable insights and practical guidelines for characterizing distinct lithium states within LMBs. 展开更多
关键词 NMR spectroscopy lithium-7 lithium metal battery Electrolyte Electrode-protective layer Solid electrolyte interface Magnetic susceptibility anisotropy lithium-metal NMR signal Diamagnetic^(7)Li NMR signal
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Ultra-homogeneous dense Ag nano layer enables long lifespan solid-state lithium metal batteries
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作者 Yaning Liu Tianqi Yang +13 位作者 Ruyi Fang Chengwei Lu Ruojian Ma Ke Yue Zhen Xiao Xiaozheng Zhou Wenkui Zhang Xinping He Yongping Gan Jun Zhang Xinhui Xia Hui Huang Xinyong Tao Yang Xia 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期110-119,共10页
The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano i... The unstable electrolyte/lithium(Li)anode interface has been one of the key challenges in realizing high energy density solid-state lithium metal batteries(LMBs)applications.Herein,a dense and uniform silver(Ag)nano interlayer with a thickness of∼35 nm is designed accurately by magnetron sputtering technology to optimize the electrolyte/Li anode interface.This Ag nano layer reacts with Li metal anode to in-situ form Li-Ag alloy,thus enhancing the physical interfacial contact,and further improving the interfacial wettability and compatibility.In particular,the Li-Ag alloy is inclined to form AgLi phase proved by cryo-TEM and DFT,effectively preventing SN from continuously“attacking”the Li metal anode due to the lower adsorption of succinonitrile(SN)molecules on AgLi than that of pure Li metal,thereby significantly reinforcing the interfacial stability.Hence,the enhanced physical and chemical stability of electrolyte/Li anode interface promotes the homogeneous deposition of Li^(+)and inhibits the dendrite growth.The Li-symmetric cell maintains stable operation for up to 1700 h and the cycling stability of LiFePO_(4)|SPE|Li full cell is remarkably improved at room temperature(capacity retention rate of 91.9%for 200 cycles).This work opens an effective way for accurate and controllable interface design of long lifespan solid-state LMBs. 展开更多
关键词 Silvernano layer Poly(ethylene oxide) Solid polymer electrolyte SUCCINONITRILE lithium metal battery
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Porous Organic Cage‑Based Quasi‑Solid‑State Electrolyte with Cavity‑Induced Anion‑Trapping Effect for Long‑Life Lithium Metal Batteries
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作者 Wei-Min Qin Zhongliang Li +7 位作者 Wen‑Xia Su Jia‑Min Hu Hanqin Zou Zhixuan Wu Zhiqin Ruan Yue‑Peng Cai Kang Li Qifeng Zheng 《Nano-Micro Letters》 SCIE EI CAS 2025年第2期376-386,共11页
Porous organic cages(POCs)with permanent porosity and excellent host–guest property hold great potentials in regulating ion transport behavior,yet their feasibility as solid-state electrolytes has never been testifie... Porous organic cages(POCs)with permanent porosity and excellent host–guest property hold great potentials in regulating ion transport behavior,yet their feasibility as solid-state electrolytes has never been testified in a practical battery.Herein,we design and fabricate a quasi-solid-state electrolyte(QSSE)based on a POC to enable the stable operation of Li-metal batteries(LMBs).Benefiting from the ordered channels and cavity-induced anion-trapping effect of POC,the resulting POC-based QSSE exhibits a high Li+transference number of 0.67 and a high ionic conductivity of 1.25×10^(−4) S cm^(−1) with a low activation energy of 0.17 eV.These allow for homogeneous Li deposition and highly reversible Li plating/stripping for over 2000 h.As a proof of concept,the LMB assembled with POC-based QSSE demonstrates extremely stable cycling performance with 85%capacity retention after 1000 cycles.Therefore,our work demonstrates the practical applicability of POC as SSEs for LMBs and could be extended to other energy-storage systems,such as Na and K batteries. 展开更多
关键词 Porous organic cage Cavity-induced anion-trapping Quasi-solid-state electrolyte Homogeneous Li+flux lithium metal battery
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Laser-Constructing 3D Copper Current Collector with Crystalline Orientation Selectivity for Stable Lithium Metal Batteries
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作者 Hui Li Gang Wang +3 位作者 Jin Hu Jun Li Jiaxu Huang Shaolin Xu 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第6期129-139,共11页
The practical application of lithium(Li)metal anodes in high-capacity batteries is impeded by the formation of hazardous Li dendrites.To address this challenge,this research presents a novel methodology that combines ... The practical application of lithium(Li)metal anodes in high-capacity batteries is impeded by the formation of hazardous Li dendrites.To address this challenge,this research presents a novel methodology that combines laser ablation and heat treatment to precisely induce controlled grain growth within laser-structured grooves on copper(Cu)current collectors.Specifically,this approach enhances the prevalence of Cu(100)facets within the grooves,effectively lowering the overpotential for Li nucleation and promoting preferential Li deposition.Unlike approaches that modify the entire surface of collectors,our work focuses on selectively enhancing lithiophilicity within the grooves to mitigate the formation of Li dendrites and exhibit exceptional performance metrics.The half-cell with these collectors maintains a remarkable Coulombic efficiency of 97.42%over 350 cycles at 1 mA cm^(−2).The symmetric cell can cycle stably for 1600 h at 0.5 mA cm^(−2).Furthermore,when integrated with LiFePO4 cathodes,the full-cell configuration demonstrates outstanding capacity retention of 92.39%after 400 cycles at a 1C discharge rate.This study introduces a novel technique for fabricating selective lithiophilic three-dimensional(3D)Cu current collectors,thereby enhancing the performance of Li metal batteries.The insights gained from this approach hold promise for enhancing the performance of all laser-processed 3D Cu current collectors by enabling precise lithiophilic modifications within complex structures. 展开更多
关键词 copper current collector heat treatment laser processing lithium metal battery selective crystalline orientation
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Interfacial fusion-enhanced 11 μm-thick gel polymer electrolyte for high-performance lithium metal batteries
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作者 Ying Jiang Xinyue Hong +3 位作者 Peng Huang Jing Shi Wen Yan Chao Lai 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第11期58-66,共9页
In the pursuit of ultrathin polymer electrolyte(<20 μm) for lithium metal batteries, achieving a balance between mechanical strength and interfacial stability is crucial for the longevity of the electrolytes.Herei... In the pursuit of ultrathin polymer electrolyte(<20 μm) for lithium metal batteries, achieving a balance between mechanical strength and interfacial stability is crucial for the longevity of the electrolytes.Herein, 11 μm-thick gel polymer electrolyte is designed via an integrated electrode/electrolyte structure supported by lithium metal anode. Benefiting from an exemplary superiority of excellent mechanical property, high ionic conductivity, and robust interfacial adhesion, the in-situ formed polymer electrolyte reinforced by titanosiloxane networks(ISPTS) embodies multifunctional roles of physical barrier, ionic carrier, and artificial protective layer at the interface. The potent interfacial interactions foster a seamless fusion of the electrode/electrolyte interfaces and enable continuous ion transport. Moreover, the built-in ISPTS electrolyte participates in the formation of gradient solid-electrolyte interphase(SEI) layer, which enhances the SEI's structural integrity against the strain induced by volume fluctuations of lithium anode.Consequently, the resultant 11 μm-thick ISPTS electrolyte enables lithium symmetric cells with cycling stability over 600 h and LiFePO_(4) cells with remarkable capacity retention of 96.6% after 800 cycles.This study provides a new avenue for designing ultrathin polymer electrolytes towards stable, safe,and high-energy–density lithium metal batteries. 展开更多
关键词 Ultrathin gel polymer electrolyte Integrated electrode/electrolyte structure Quasi-solid-state lithium metal battery Solid-electrolyte interphase
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In-situ electro-polymerization of L-tyrosine enables ultrafast,long cycle life for lithium metal battery
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作者 Zihao Chu Sidong Zhuang +3 位作者 Jiahui Lu Jiabao Li Chengyin Wang Tianyi Wang 《Chinese Chemical Letters》 SCIE CAS CSCD 2023年第5期561-566,共6页
The growth of dendrites in the lithium(Li)metal anode hinders the commercialization of lithium metal batteries(LMBs).Electrolyte additives have proved to be an effective way to solve the problem of dendrites and impro... The growth of dendrites in the lithium(Li)metal anode hinders the commercialization of lithium metal batteries(LMBs).Electrolyte additives have proved to be an effective way to solve the problem of dendrites and improve the coulombic efficiency.Herein,we propose a strategy of using L-tyrosine(L-Tyr)as an additive to protect the lithium metal anode in situ,where L-Tyr can be electropolymerized in situ to form an ordered array of nanosheets on the surface of the lithium metal anode to uniformly deposit lithium ions.At the same time,the addition of L-Tyr changed the structure of the solvent in the electrolyte,because the carboxyl group on L-Tyr make DME form hydrogen bonds easily.Besides,the reduction of free DME makes more TFSI-involved in the formation of the SEI film on the electrode surface,which increases the proportion of LiF in the SEI film.With 2 wt%L-Tyr,Li||Li symmetric cells superior cycle stability in ether electrolytes,Li|Cu cells y improved stability up to 200 cycles with an average CE of 93.1%in ether electrolytes and Li||Li_(4)Ti_(5)O_(12)(LTO)demonstrated an excellent cycling capabilitie with 119 mAh/g capacity retention by the 5000^(th)cycle. 展开更多
关键词 lithium metal battery TYROSINE In situ Eelectropolymerization lithium dendrite
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