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Unique double-layer solid electrolyte interphase formed with fluorinated ether-based electrolytes for high-voltage lithium metal batteries 被引量:2
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作者 Ruo Wang Jiawei Li +11 位作者 Bing Han Qingrong Wang Ruohong Ke Tong Zhang Xiaohu Ao Guangzhao Zhang Zhongbo Liu Yunxian Qian Fangfang Pan Iseult Lynch Jun Wang Yonghong Deng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期532-542,I0012,共12页
Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the... Li metal batteries using high-voltage layered oxides cathodes are of particular interest due to their high energy density.However,they suffer from short lifespan and extreme safety concerns,which are attributed to the degradation of layered oxides and the decomposition of electrolyte at high voltage,as well as the high reactivity of metallic Li.The key is the development of stable electrolytes against both highvoltage cathodes and Li with the formation of robust interphase films on the surfaces.Herein,we report a highly fluorinated ether,1,1,1-trifluoro-2-[(2,2,2-trifluoroethoxy)methoxy]ethane(TTME),as a cosolvent,which not only functions as a diluent forming a localized high concentration electrolyte(LHCE),but also participates in the construction of the inner solvation structure.The TTME-based electrolyte is stable itself at high voltage and induces the formation of a unique double-layer solid electrolyte interphase(SEI)film,which is embodied as one layer rich in crystalline structural components for enhanced mechanical strength and another amorphous layer with a higher concentration of organic components for enhanced flexibility.The Li||Cu cells display a noticeably high Coulombic efficiency of 99.28%after 300 cycles and Li symmetric cells maintain stable cycling more than 3200 h at 0.5 mA/cm^(2) and 1.0m Ah/cm^(2).In addition,lithium metal cells using LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) and Li CoO_(2) cathodes(both loadings~3.0 m Ah/cm^(2))realize capacity retentions of>85%over 240 cycles with a charge cut-off voltage of 4.4 V and 90%for 170 cycles with a charge cut-off voltage of 4.5 V,respectively.This study offers a bifunctional ether-based electrolyte solvent beneficial for high-voltage Li metal batteries. 展开更多
关键词 Lithium metal batteries High-voltage layered oxides Fluorinated ether-based electrolytes solid electrolyte interphase Cathode electrolyte interphase
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How Does Stacking Pressure Affect the Performance of Solid Electrolytes and All-Solid-State Lithium Metal Batteries? 被引量:2
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作者 Junwu Sang Bin Tang +3 位作者 Yong Qiu Yongzheng Fang Kecheng Pan Zhen Zhou 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第4期93-98,共6页
All-solid-state lithium metal batteries(ASSLMBs)with solid electrolytes(SEs)have emerged as a promising alternative to liquid electrolyte-based Li-ion batteries due to their higher energy density and safety.However,si... All-solid-state lithium metal batteries(ASSLMBs)with solid electrolytes(SEs)have emerged as a promising alternative to liquid electrolyte-based Li-ion batteries due to their higher energy density and safety.However,since ASSLMBs lack the wetting properties of liquid electrolytes,they require stacking pressure to prevent contact loss between electrodes and SEs.Though previous studies showed that stacking pressure could impact certain performance aspects,a comprehensive investigation into the effects of stacking pressure has not been conducted.To address this gap,we utilized the Li_(6)PS_(5)Cl solid electrolyte as a reference and investigated the effects of stacking pressures on the performance of SEs and ASSLMBs.We also developed models to explain the underlying origin of these effects and predict battery performance,such as ionic conductivity and critical current density.Our results demonstrated that an appropriate stacking pressure is necessary to achieve optimal performance,and each step of applying pressure requires a specific pressure value.These findings can help explain discrepancies in the literature and provide guidance to establish standardized testing conditions and reporting benchmarks for ASSLMBs.Overall,this study contributes to the understanding of the impact of stacking pressure on the performance of ASSLMBs and highlights the importance of careful pressure optimization for optimal battery performance. 展开更多
关键词 critical current density solid electrolyte solid-state lithium metal batteries stacking pressure
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Borohydride Ammoniate Solid Electrolyte Design for All-Solid-State Mg Batteries 被引量:1
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作者 Yuepeng Pang Zhengfang Nie +5 位作者 Fen Xu Lixian Sun Junhe Yang Dalin Sun Fang Fang Shiyou Zheng 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第1期100-106,共7页
Searching for novel solid electrolytes is of great importance and challenge for all-solid-state Mg batteries.In this work,we develop an amorphous Mg borohydride ammoniate,Mg(BH_(4))_(2)·2NH_(3),as a solid Mg elec... Searching for novel solid electrolytes is of great importance and challenge for all-solid-state Mg batteries.In this work,we develop an amorphous Mg borohydride ammoniate,Mg(BH_(4))_(2)·2NH_(3),as a solid Mg electrolyte that prepared by a NH_(3)redistribution between 3D framework-γ-Mg(BH_(4))_(2)and Mg(BH_(4))_(2)·6NH_(3).Amorphous Mg(BH_(4))_(2)·2NH_(3)exhibits a high Mg-ion conductivity of 5×10^(-4)S cm^(-1)at 75℃,which is attributed to the fast migration of abundant Mg vacancies according to the theoretical calculations.Moreover,amorphous Mg(BH_(4))_(2)·2NH_(3)shows an apparent electrochemical stability window of 0-1.4 V with the help of in-situ formed interphases,which can prevent further side reactions without hindering the Mg-ion transfer.Based on the above superiorities,amorphous Mg(BH_(4))_(2)·2NH_(3)enables the stable cycling of all-solid-state Mg cells,as the critical current density reaches 3.2 mA cm^(-2)for Mg symmetrical cells and the reversible specific capacity reaches 141 mAh g^(-1)with a coulombic efficiency of 91.7%(first cycle)for Mg||TiS_(2)cells. 展开更多
关键词 all-solid-state Mg batteries amorphization Mg borohydride ammoniate Mg vacancy migration solid electrolyte
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Construction of a High‑Performance Composite Solid Electrolyte Through In‑Situ Polymerization within a Self‑Supported Porous Garnet Framework 被引量:1
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作者 An‑Giang Nguyen Min‑Ho Lee +1 位作者 Jaekook Kim Chan‑Jin Park 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第5期56-70,共15页
Composite solid electrolytes(CSEs)have emerged as promising candidates for safe and high-energy–density solid-state lithium metal batteries(SSLMBs).However,concurrently achieving exceptional ionic conductivity and in... Composite solid electrolytes(CSEs)have emerged as promising candidates for safe and high-energy–density solid-state lithium metal batteries(SSLMBs).However,concurrently achieving exceptional ionic conductivity and interface compatibility between the electrolyte and electrode presents a significant challenge in the development of high-performance CSEs for SSLMBs.To overcome these challenges,we present a method involving the in-situ polymerization of a monomer within a self-supported porous Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZT)to produce the CSE.The synergy of the continuous conductive LLZT network,well-organized polymer,and their interface can enhance the ionic conductivity of the CSE at room temperature.Furthermore,the in-situ polymerization process can also con-struct the integration and compatibility of the solid electrolyte–solid electrode interface.The synthesized CSE exhibited a high ionic conductivity of 1.117 mS cm^(-1),a significant lithium transference number of 0.627,and exhibited electrochemical stability up to 5.06 V vs.Li/Li+at 30℃.Moreover,the Li|CSE|LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2) cell delivered a discharge capacity of 105.1 mAh g^(-1) after 400 cycles at 0.5 C and 30℃,corresponding to a capacity retention of 61%.This methodology could be extended to a variety of ceramic,polymer electrolytes,or battery systems,thereby offering a viable strategy to improve the electrochemical properties of CSEs for high-energy–density SSLMBs. 展开更多
关键词 Scalable tape-casting method Self-supported porous Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12) Composite solid electrolyte LiF-and B-rich interphase layers
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Overcoming the Na-ion conductivity bottleneck for the cost-competitive chloride solid electrolytes
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作者 Lv Hu Hui Li +3 位作者 Fang Chen Yating Liu Jinzhu Wang Cheng Ma 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期1-8,I0001,共9页
Chloride solid electrolytes possess multiple advantages for the construction of safe,energy-dense allsolid-state sodium batteries,but presently the chlorides with sufficiently high cost-competitiveness for commerciali... Chloride solid electrolytes possess multiple advantages for the construction of safe,energy-dense allsolid-state sodium batteries,but presently the chlorides with sufficiently high cost-competitiveness for commercialization almost all exhibit low Na-ion conductivities of around 10^(-5)S cm^(-1)or lower.Here,we report a chloride solid electrolyte,Na_(2.7)ZFCl_(5.3)O_(0.7),which reaches a Na-ion conductivity of 2.29×10^(-4)S cm^(-1)at 25℃without involving overly expensive raw materials such as rare-earth chlorides or Na_(2)S.In addition to the efficient ion transport,Na_(2.7)ZrCl_(5.3)O_(0.7)also shows an excellent deformability surpassing that of the widely studied Na_(3)PS_(4),Na_(3)SbS_(4),and Na_(2)ZrCl_(6)solid electrolytes.The combination of these advantages allows the all-solid-state cell based on Na_(2.7)ZrCl_(5.3)O_(0.7)and NaCrO_(2)to realize stable room-temperature cycling at a much higher specific current than those based on other non-viscoelastic chloride solid electrolytes in literature(120 mA g^(-1)vs.12-55 mA g^(-1));after 100 cycles at such a high rate,the Na_(2.7)ZFCl_(5.3)O_(0.7)-based cell can still deliver a discharge capacity of 80 mAh g^(-1)at25℃. 展开更多
关键词 All-solid-state sodium batteries Ionic conductivities solid electrolytes Chlorides High voltage stability
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PDOL-Based Solid Electrolyte Toward Practical Application:Opportunities and Challenges
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作者 Hua Yang Maoxiang Jing +3 位作者 Li Wang Hong Xu Xiaohong Yan Xiangming He 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第7期109-141,共33页
Polymer solid-state lithium batteries(SSLB)are regarded as a promising energy storage technology to meet growing demand due to their high energy density and safety.Ion conductivity,interface stability and battery asse... Polymer solid-state lithium batteries(SSLB)are regarded as a promising energy storage technology to meet growing demand due to their high energy density and safety.Ion conductivity,interface stability and battery assembly process are still the main challenges to hurdle the commercialization of SSLB.As the main component of SSLB,poly(1,3-dioxolane)(PDOL)-based solid polymer electrolytes polymerized in-situ are becoming a promising candidate solid elec-trolyte,for their high ion conductivity at room temperature,good battery elec-trochemical performances,and simple assembly process.This review analyzes opportunities and challenges of PDOL electrolytes toward practical application for polymer SSLB.The focuses include exploring the polymerization mechanism of DOL,the performance of PDOL composite electrolytes,and the application of PDOL.Furthermore,we provide a perspective on future research directions that need to be emphasized for commercialization of PDOL-based electrolytes in SSLB.The exploration of these schemes facilitates a comprehensive and profound understanding of PDOL-based polymer electrolyte and provides new research ideas to boost them toward practical application in solid-state batteries. 展开更多
关键词 Poly(1 3-dioxolane) solid electrolyte Polymerization mechanism Composite electrolyte Practical application
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Regulating solid electrolyte interphase film on fluorinedoped hard carbon anode for sodium-ion battery
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作者 Cuiyun Yang Wentao Zhong +4 位作者 Yuqiao Liu Qiang Deng Qian Cheng Xiaozhao Liu Chenghao Yang 《Carbon Energy》 SCIE EI CAS CSCD 2024年第6期200-215,共16页
For the performance optimization strategies of hard carbon,heteroatom doping is an effective way to enhance the intrinsic transfer properties of sodium ions and electrons for accelerating the reaction kinetics.However... For the performance optimization strategies of hard carbon,heteroatom doping is an effective way to enhance the intrinsic transfer properties of sodium ions and electrons for accelerating the reaction kinetics.However,the previous work focuses mainly on the intrinsic physicochemical property changes of the material,but little attention has been paid to the resulting interfacial regulation of the electrode surface,namely the formation of solid electrolyte interphase(SEI)film.In this work,element F,which has the highest electronegativity,was chosen as the doping source to,more effectively,tune the electronic structure of the hard carbon.The effect of F-doping on the physicochemical properties of hard carbon was not only systematically analyzed but also investigated with spectroscopy,optics,and in situ characterization techniques to further verify that appropriate F-doping plays a positive role in constructing a homogenous and inorganic-rich SEI film.The experimentally demonstrated link between the electronic structure of the electrode and the SEI film properties can reframe the doping optimization strategy as well as provide a new idea for the design of electrode materials with low reduction kinetics to the electrolyte.As a result,the optimized sample with the appropriate F-doping content exhibits the best electrochemical performance with high capacity(434.53 mA h g^(-1)at 20mA g^(-1))and excellent rate capability(141 mAh g^(-1)at 400 mA g^(-1)). 展开更多
关键词 F-doping hard carbon reduction kinetics sodium-ion batteries solid electrolyte interphase film
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Advancements and Challenges in Organic–Inorganic Composite Solid Electrolytes for All‑Solid‑State Lithium Batteries
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作者 Xueyan Zhang Shichao Cheng +4 位作者 Chuankai Fu Geping Yin Liguang Wang Yongmin Wu Hua Huo 《Nano-Micro Letters》 SCIE EI CAS 2025年第1期46-97,共52页
To address the limitations of contemporary lithium-ion batteries,particularly their low energy density and safety concerns,all-solid-state lithium batteries equipped with solid-state electrolytes have been identified ... To address the limitations of contemporary lithium-ion batteries,particularly their low energy density and safety concerns,all-solid-state lithium batteries equipped with solid-state electrolytes have been identified as an up-and-coming alternative.Among the various SEs,organic–inorganic composite solid electrolytes(OICSEs)that combine the advantages of both polymer and inorganic materials demonstrate promising potential for large-scale applications.However,OICSEs still face many challenges in practical applications,such as low ionic conductivity and poor interfacial stability,which severely limit their applications.This review provides a comprehensive overview of recent research advancements in OICSEs.Specifically,the influence of inorganic fillers on the main functional parameters of OICSEs,including ionic conductivity,Li+transfer number,mechanical strength,electrochemical stability,electronic conductivity,and thermal stability are systematically discussed.The lithium-ion conduction mechanism of OICSE is thoroughly analyzed and concluded from the microscopic perspective.Besides,the classic inorganic filler types,including both inert and active fillers,are categorized with special emphasis on the relationship between inorganic filler structure design and the electrochemical performance of OICSEs.Finally,the advanced characterization techniques relevant to OICSEs are summarized,and the challenges and perspectives on the future development of OICSEs are also highlighted for constructing superior ASSLBs. 展开更多
关键词 Composite solid electrolytes Inorganic filler Interfacial stability Li-ion conduction mechanism Characterization techniques
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In situ high-quality LiF/Li_(3)N inorganic and phenyl-based organic solid electrolyte interphases for advanced lithium–oxygen batteries
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作者 Qianyan Wang Minsheng Wu +7 位作者 Yunkai Xu Chuyue Li Yuanjia Rong Yaling Liao Menglin Gao Xiaoping Zhang Weirong Chen Jun Lu 《Carbon Energy》 SCIE EI CAS CSCD 2024年第9期29-38,共10页
Lithium metal shows a great advantage as the most promising anode for its unparalleled theoretical specific capacity and extremely low electrochemical potential.However,uncontrolled lithium dendrite growth and severe ... Lithium metal shows a great advantage as the most promising anode for its unparalleled theoretical specific capacity and extremely low electrochemical potential.However,uncontrolled lithium dendrite growth and severe side reactions of the reactive intermediates and organic electrolytes still limit the broad application of lithium metal batteries.Herein,we propose 4-nitrobenzenesulfonyl fluoride(NBSF)as an electrolyte additive for forming a stable organic-inorganic hybrid solid electrolyte interphase(SEI)layer on the lithium surface.The abundance of lithium fluoride and lithium nitride can guarantee the SEI layer's toughness and high ionic conductivity,achieving dendrite-free lithium deposition.Meanwhile,the phenyl group of NBSF significantly contributes to both the chemical stability of the SEI layer and the good adaptation to volume changes of the lithium anode.The lithium-oxygen batteries with NBSF exhibit prolonged cycle lives and excellent cycling stability.This simple approach is hoped to improve the development of the organic-inorganic SEI layer to stabilize the lithium anodes for lithium-oxygen batteries. 展开更多
关键词 lithium anode lithium-oxygen batteries reactive oxygen species solid electrolyte interphase
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Reasonable design a high-entropy garnet-type solid electrolyte for all-solid-state lithium batteries
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作者 Shiyu Yu Yandi Li +6 位作者 Jiaxin Luo Daming Chen Liang Yang Yaqing Wei De Li Yuanxun Li Yong Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期414-423,共10页
Traditional garnet solid electrolyte(Li_(7)La_(3)Zr_(2)O_(12))suffers from low room temperature ionic conductivity,poor air stability,high sintering temperature and energy consumption.Considering the development prosp... Traditional garnet solid electrolyte(Li_(7)La_(3)Zr_(2)O_(12))suffers from low room temperature ionic conductivity,poor air stability,high sintering temperature and energy consumption.Considering the development prospects of high-entropy materials with high structural disorder and strong component controllability in the field of electrochemical energy storage,herein,a novel high-entropy garnet-type oxide solid electrolyte,Li_(5.75)Ga_(0.25)La_(3)Zr_(0.5)Ti_(0.5)Sn_(0.5)Nb_(0.5)O_(12)(LGLZTSNO)was constructed by partially replacing the Li and Zr sites in Li_(7)La_(3)Zr_(2)O_(12)with Ga and Ti/Sn/Nb elements,respectively.The experimental and density functional theory(DFT)calculation results show that the high-entropy LGLZTSNO electrolyte has preferable room temperature ion conductivity,air stability,interface contact performance with lithium anode,and the ability to suppress lithium dendrites.Thanks to the improvement of electrolyte performance,the critical current density of Li/Ag@LGLZTSNO/Li symmetric cell was increased from 0.42 to 1.57 mA cm^(−2),and the interface area specific impedance(IASR)was reduced from 765.2 to 42.3Ωcm^(2).Meanwhile,the Li/Ag@LGLZTSNO/LFP full cell also exhibits excellent rate performance and cycling performance(148 mA h g^(−1)at 0.1 C and 124 mA h g^(−1)at 0.5 C,capacity retention up to 84.8%after 100 cycles at 0.1 C),showing the application prospects of high-entropy LGLZTSNO solid electrolyte in high-performance all solid state lithium batteries. 展开更多
关键词 Garnet solid electrolyte Dual-site substitution High-entropy all solid-state lithium batteries(ASSLBs)
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Synergistic coupling among Mg_(2)B_(2)O_(5),polycarbonate and N,Ndimethylformamide enhances the electrochemical performance of PVDF-HFP-based solid electrolyte
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作者 Yutong Jing Qiang Lv +8 位作者 Yujia Chen Bo Wang Bochen Wu Cheng Li Shengbo Yang Zhipeng He Dianlong Wang Huakun Liu Shixue Dou 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第7期158-168,共11页
Polymer solid electrolytes(SPEs)based on the[solvate-Li+]complex structure have promising prospects in lithium metal batteries(LMBs)due to their unique ion transport mechanism.However,the solvation structure may compr... Polymer solid electrolytes(SPEs)based on the[solvate-Li+]complex structure have promising prospects in lithium metal batteries(LMBs)due to their unique ion transport mechanism.However,the solvation structure may compromise the mechanical performance and safety,hindering practical application of SPEs.In this work,a composite solid electrolyte(CSE)is designed through the organic-inorganic syner-gistic interaction among N,N-dimethylformamide(DMF),polycarbonate(PC),and Mg_(2)B_(2)O_(5) in poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP).Flame-retardant Mg_(2)B_(2)O_(5) nanowires provide non-flammability to the prepared CSEs,and the addition of PC improves the dispersion of Mg_(2)B_(2)O_(5) nanowires.Simultaneously,the organic-inorganic synergistic action of PC plasticizer and Mg_(2)B_(2)O_(5) nanowires pro-motes the dissociation degree of LiTFSI and reduces the crystallinity of PVDF-HFP,enabling rapid Li ion transport.Additionally,Raman spectroscopy and DFT calculations confirm the coordination between Mg atoms in Mg_(2)B_(2)O_(5) and N atoms in DMF,which exhibits Lewis base-like behavior attacking adjacent C-F and C-H bonds in PVDF-HFP while inducing dehydrofluorination of PVDF-HFP.Based on the syner-gistic coupling of Mg_(2)B_(2)O_(5),PC,and DMF in the PVDF-HFP matrix,the prepared CSE exhibits superior ion conductivity(9.78×10^(-4) s cm^(-1)).The assembled Li symmetric cells cycle stably for 3900 h at a current density of 0.1 mA cm^(-2) without short circuit.The LFP||Li cells assembled with PDL-Mg_(2)B_(2)O_(5)/PC CSEs show excellent rate capability and cycling performance,with a capacity retention of 83.3%after 1000 cycles at 0.5 C.This work provides a novel approach for the practical application of organic-inorganic Synergistic CSEs in LMBs. 展开更多
关键词 Composite solid electrolytes Safe Li metal batteries Synergistic coupling effect Poly(vinylidene fluoride-co-hexafluoropro pylene)
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Synergetic Control of Li^(+)Transport Ability and Solid Electrolyte Interphase by Boron-Rich Hexagonal Skeleton Structured All-Solid-State Polymer Electrolyte
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作者 Yanan Li Shunchao Ma +7 位作者 Yuehua Zhao Silin Chen Tingting Xiao Hongxing Yin Huiyu Song Xiumei Pan Lina Cong Haiming Xie 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第3期154-163,共10页
High Li^(+)transference number electrolytes have long been understood to provide attractive candidates for realizing uniform deposition of Li^(+).However,such electrolytes with immobilized anions would result in incom... High Li^(+)transference number electrolytes have long been understood to provide attractive candidates for realizing uniform deposition of Li^(+).However,such electrolytes with immobilized anions would result in incomplete solid electrolyte interphase(SEI)formation on the Li anode because it suffers from the absence of appropriate inorganic components entirely derived from anions decomposition.Herein,a boron-rich hexagonal polymer structured all-solid-state polymer electrolyte(BSPE+10%LiBOB)with regulated intermolecular interaction is proposed to trade off a high Li^(+)transference number against stable SEI properties.The Li^(+)transference number of the as-prepared electrolyte is increased from 0.23 to 0.83 owing to the boron-rich cross-linker(BC)addition.More intriguingly,for the first time,the experiments combined with theoretical calculation results reveal that BOB^(-)anions have stronger interaction with B atoms in polymer chain than TFSI^(-),which significantly induce the TFSI^(-)decomposition and consequently increase the amount of LiF and Li3N in the SEI layer.Eventually,a LiFePO_(4)|BSPE+10%LiBOBlLi cell retains 96.7%after 400 cycles while the cell without BC-resisted electrolyte only retains 40.8%.BSPE+10%LiBOB also facilitates stable electrochemical cycling of solid-state Li-S cells.This study blazes a new trail in controlling the Li^(+)transport ability and SEI properties,synergistically. 展开更多
关键词 all-solid-state electrolyte boron-rich polymer lithium metal batteries lithium-ion transference number solid electrolyte interphase layer
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Theoretical Design of Defects as a Driving Force for Ion Transport in Li_(3)OBr Solid Electrolyte
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作者 Xingyun Luo Yanlu Li Xian Zhao 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第3期143-153,共11页
Due to ever-increasing concerns about safety issues in using Li ionic batteries,solid electrolytes have extensively explored.The Li-rich antiperovskite Li_(3)OBr has been considered as a promising solid electrolyte ca... Due to ever-increasing concerns about safety issues in using Li ionic batteries,solid electrolytes have extensively explored.The 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 lattice.Herein,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 theoretically.It 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 boundaries.The 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 crystal.This work provides a comprehensive insight into the Li^(+)transport and conduction mechanism in the Li_(3)OBr electrolyte.It opens a new way of improving the conductivity for all-solid-state Li electrolyte material through the defect design. 展开更多
关键词 DEFECTS density functional theory ionic migration solid electrolyte
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Synthesis of High Purity Lithium Sulfide for Sulfide Solid Electrolyte Applications through Hydrogen Reduction of Lithium Sulfate
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作者 Arafumi Kimura 《陶瓷学报》 CAS 北大核心 2024年第4期689-695,共7页
This paper is aimed to present a clean,inexpensive and sustainable method to synthesize high purity lithium sulfide(Li_(2)S)powder through hydrogen reduction of lithium sulfate(Li_(2)SO_(4)).A three-step reduction pro... This paper is aimed to present a clean,inexpensive and sustainable method to synthesize high purity lithium sulfide(Li_(2)S)powder through hydrogen reduction of lithium sulfate(Li_(2)SO_(4)).A three-step reduction process has been successfully developed to synthesize well-crystallized and single-phase Li_(2)S powder by investigating the melting,sintering and reduction behavior of the mixtures of Li_(2)SO_(4)-Li_(2)S.High purity alumina was found to be the most suitable crucible material for producing high purity Li_(2)S,because it was not attacked by the Li_(2)SO_(4)-Li_(2)S melt during heating,as compared with other materials,such as carbon,mullite,quartz,boron nitride and stainless steel.The use of synthesized LizS resulted in higher purity and substantially higher room temperature ionic conductivity(2.77 mS·cm^(-1))for the argyrodite sulfide electrolyte Li_(6)PS_(5)Cl than commercial Li_(2)S(1.12 mS·cm^(-1)).This novel method offers a great opportunity to produce battery grade Li_(2)S for sulfide solid electrolyte applications. 展开更多
关键词 lithium sulfide lithium sulfate hydrogen reduction sulfide solid electrolyte all-solid-state lithium-ion battery
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A critical review on composite solid electrolytes for lithium batteries:Design strategies and interface engineering 被引量:2
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作者 Tianqi Yang Cheng Wang +7 位作者 Wenkui Zhang Yang Xia Hui Huang Yongping Gan Xinping He Xinhui Xia Xinyong Tao Jun Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第9期189-209,共21页
The rapid development of new energy vehicles and 5G communication technologies has led to higher demands for the safety,energy density,and cycle performance of lithium-ion batteries as power sources.However,the curren... The rapid development of new energy vehicles and 5G communication technologies has led to higher demands for the safety,energy density,and cycle performance of lithium-ion batteries as power sources.However,the currently used liquid carbonate compounds in commercial lithium-ion battery electrolytes pose potential safety hazards such as leakage,swelling,corrosion,and flammability.Solid electrolytes can be used to mitigate these risks and create a safer lithium battery.Furthermore,high-energy density can be achieved by using solid electrolytes along with high-voltage cathode and metal lithium anode.Two types of solid electrolytes are generally used:inorganic solid electrolytes and polymer solid electrolytes.Inorganic solid electrolytes have high ionic conductivity,electrochemical stability window,and mechanical strength,but suffer from large solid/solid contact resistance between the electrode and electrolyte.Polymer solid electrolytes have good flexibility,processability,and contact interface properties,but low room temperature ionic conductivity,necessitating operation at elevated temperatures.Composite solid electrolytes(CSEs) are a promising alternative because they offer light weight and flexibility,like polymers,as well as the strength and stability of inorganic electrolytes.This paper presents a comprehensive review of recent advances in CSEs to help researchers optimize CSE composition and interactions for practical applications.It covers the development history of solid-state electrolytes,CSE properties with respect to nanofillers,morphology,and polymer types,and also discusses the lithium-ion transport mechanism of the composite electrolyte,and the methods of engineering interfaces with the positive and negative electrodes.Overall,the paper aims to provide an outlook on the potential applications of CSEs in solid-state lithium batteries,and to inspire further research aimed at the development of more systematic optimization strategies for CSEs. 展开更多
关键词 Inorganic solid electrolytes Polymer solid electrolytes Composite solid electrolytes Interface engineering
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In-situ polymerized PEO-based solid electrolytes contribute better Li metal batteries:Challenges,strategies,and perspectives
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作者 Zhihui Jia Yong Liu +4 位作者 Haoming Li Yi Xiong Yingjie Miao Zhongxiu Liu Fengzhang Ren 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期548-571,共24页
Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)with good electrochemical stability and excellent Li salt solubility are considered as one of the most promising SPEs for solid-state lithium metal batteri... Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)with good electrochemical stability and excellent Li salt solubility are considered as one of the most promising SPEs for solid-state lithium metal batteries(SSLMBs).However,PEO-based SPEs suffer from low ionic conductivity at room temperature and high interfacial resistance with the electrodes due to poor interfacial contact,seriously hindering their practical applications.As an emerging technology,in-situ polymerization process has been widely used in PEO-based SPEs because it can effectively increase Li-ion transport at the interface and improve the interfacial contact between the electrolyte and electrodes.Herein,we review recent advances in design and fabrication of in-situ polymerized PEO-based SPEs to realize enhanced performance in LMBs.The merits and current challenges of various SPEs,as well as their stabilizing strategies are presented.Furthermore,various in-situ polymerization methods(such as free radical polymerization,cationic polymerization,anionic polymerization)for the preparation of PEO-based SPEs are summarized.In addition,the application of in-situ polymerization technology in PEO-based SPEs for adjustment of the functional units and addition of different functional filler materials was systematically discussed to explore the design concepts,methods and working mechanisms.Finally,the challenges and future prospects of in-situ polymerized PEO-based SPEs for SSLMBs are also proposed. 展开更多
关键词 In-situ polymerization Polyethylene oxide solid polymer electrolytes Lithium metal anodes
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Rational Design of High-Performance PEO/Ceramic Composite Solid Electrolytes for Lithium Metal Batteries 被引量:7
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作者 Yanxia Su Fei Xu +2 位作者 Xinren Zhang Yuqian Qiu Hongqiang Wang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第6期155-189,共35页
Composite solid electrolytes(CSEs)with poly(ethylene oxide)(PEO)have become fairly prevalent for fabricating high-performance solid-state lithium metal batteries due to their high Li~+solvating capability,flexible pro... Composite solid electrolytes(CSEs)with poly(ethylene oxide)(PEO)have become fairly prevalent for fabricating high-performance solid-state lithium metal batteries due to their high Li~+solvating capability,flexible processability and low cost.However,unsatisfactory room-temperature ionic conductivity,weak interfacial compatibility and uncontrollable Li dendrite growth seriously hinder their progress.Enormous efforts have been devoted to combining PEO with ceramics either as fillers or major matrix with the rational design of two-phase architecture,spatial distribution and content,which is anticipated to hold the key to increasing ionic conductivity and resolving interfacial compatibility within CSEs and between CSEs/electrodes.Unfortunately,a comprehensive review exclusively discussing the design,preparation and application of PEO/ceramic-based CSEs is largely lacking,in spite of tremendous reviews dealing with a broad spectrum of polymers and ceramics.Consequently,this review targets recent advances in PEO/ceramicbased CSEs,starting with a brief introduction,followed by their ionic conduction mechanism,preparation methods,and then an emphasis on resolving ionic conductivity and interfacial compatibility.Afterward,their applications in solid-state lithium metal batteries with transition metal oxides and sulfur cathodes are summarized.Finally,a summary and outlook on existing challenges and future research directions are proposed. 展开更多
关键词 Composite solid electrolytes Ionic conductivity Interfacial compatibility Ion conduction pathways Li metal batteries
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Engineering homotype heterojunctions in hard carbon to induce stable solid electrolyte interfaces for sodium-ion batteries 被引量:5
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作者 Chengxin Yu Yu Li +6 位作者 Haixia Ren Ji Qian Shuo Wang Xin Feng Mingquan Liu Ying Bai Chuan Wu 《Carbon Energy》 SCIE CAS CSCD 2023年第1期181-193,共13页
Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this ... Developing effective strategies to improve the initial Coulombic efficiency(ICE)and cycling stability of hard carbon(HC)anodes for sodium-ion batteries is the key to promoting the commercial application of HC.In this paper,homotype heterojunctions are designed on HC to induce the generation of stable solid electrolyte interfaces,which can effectively increase the ICE of HC from 64.7%to 81.1%.The results show that using a simple surface engineering strategy to construct a homotypic amorphous Al_(2)O_(3) layer on the HC could shield the active sites,and further inhibit electrolyte decomposition and side effects occurrence.Particularly,due to the suppression of continuous decomposition of NaPF 6 in ester-based electrolytes,the accumulation of NaF could be reduced,leading to the formation of thinner and denser solid electrolyte interface films and a decrease in the interface resistance.The HC anode can not only improve the ICE but elevate its sodium storage performance based on this homotype heterojunction composed of HC and Al_(2)O_(3).The optimized HC anode exhibits an outstanding reversible capacity of 321.5mAhg^(−1) at 50mAg^(−1).The cycling stability is also improved effectively,and the capacity retention rate is 86.9%after 2000 cycles at 1Ag^(−1) while that of the untreated HC is only 52.6%.More importantly,the improved sodium storage behaviors are explained by electrochemical kinetic analysis. 展开更多
关键词 hard carbon anodes homotype heterojunctions sodium-ion batteries solid electrolyte interface surface engineering
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In situ construction of a stable composite solid electrolyte interphase for dendrite-free Zn batteries 被引量:2
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作者 Yiming Zhao Huanyan Liu +4 位作者 Yu Huyan Da Lei Na Li Shan Tian Jian-Gan Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第4期450-458,共9页
Building a stable solid electrolyte interphase(SEI)has been regarded to be highly effective for mitigating the dendrite growth and parasitic side reactions of Zn anodes.Herein,a robust inorganic composite SEI layer is... Building a stable solid electrolyte interphase(SEI)has been regarded to be highly effective for mitigating the dendrite growth and parasitic side reactions of Zn anodes.Herein,a robust inorganic composite SEI layer is in situ constructed by introducing an organic cysteine additive to achieve long lifetime Zn metal batteries.The chemisorbed cysteine derivatives are electrochemically reduced to trigger a local alkaline environment for generating a gradient layered zinc hydroxide based multicomponent interphase.Such a unique interphase is of significant advantage as a corrosion inhibitor and Zn^(2+)modulator to enable reversible plating/stripping chemistry with a reduced desolvation energy barrier.Accordingly,the cells with a thin glass fiber separator(260μm)deliver a prolonged lifespan beyond 2000 h and enhanced Coulombic efficiency of 99.5%over 450 cycles.This work will rationally elaborate in situ construction of a desirable SEI by implanting reductive additives for dendrite-free Zn anodes. 展开更多
关键词 Zn metal anode electrolyte additive solid electrolyte interphase Aqueous Zn batteries
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Electrode-compatible fluorine-free multifunctional additive regulating solid electrolyte interphase and solvation structure for high-performance lithium-ion batteries 被引量:1
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作者 Qing-Song Liu Yi-Zhou Quan +4 位作者 Mei-Chen Liu Guo-Rui Zhu Xiu-Li Wang Gang Wu Yu-Zhong Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第8期239-246,I0008,共9页
The rapid development and widespread application of lithium-ion batteries(LIBs) have increased demand for high-safety and high-performance LIBs. Accordingly, various additives have been used in commercial liquid elect... The rapid development and widespread application of lithium-ion batteries(LIBs) have increased demand for high-safety and high-performance LIBs. Accordingly, various additives have been used in commercial liquid electrolytes to severally adjust the solvation structure of lithium ions, control the components of solid electrolyte interphase, or reduce flammability. While it is highly desirable to develop low-cost multifunctional electrolyte additives integrally that address both safety and performance on LIBs, significant challenges remain. Herein, a novel phosphorus-containing organic small molecule, bis(2-methoxyethyl) methylphosphonate(BMOP), was rationally designed to serve as a fluorine-free and multifunctional additive in commercial electrolytes. This novel electrolyte additive is low-toxicity,high-efficiency, low-cost, and electrode-compatible, which shows the significant improvement to both electrochemical performance and fire safety for LIBs through regulating the electrolyte solvation structure, constructing the stable electrode-electrolyte interphase, and suppressing the electrolyte combustion. This work provides a new avenue for developing safer and high-performance LIBs. 展开更多
关键词 Multifunctional additives Electrode compatibility solid electrolyte interface Solvation structure Lithium-ion batteries
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