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Trend of Developing Aqueous Liquid and Gel Electrolytes for Sustainable,Safe,and High‑Performance Li‑Ion Batteries 被引量:2
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作者 Donghwan Ji Jaeyun Kim 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第1期17-34,共18页
Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery... Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery damage or fracture is a critical concern.Water-based(aqueous)electrolytes have been receiving attention as an alternative to organic electrolytes.However,a narrow electrochemicalstability window,water decomposition,and the consequent low battery operating voltage and energy density hinder the practical use of aqueous electrolytes.Therefore,developing novel aqueous electrolytes for sustainable,safe,high-performance LIBs remains challenging.This Review first commences by summarizing the roles and requirements of electrolytes–separators and then delineates the progression of aqueous electrolytes for LIBs,encompassing aqueous liquid and gel electrolyte development trends along with detailed principles of the electrolytes.These aqueous electrolytes are progressed based on strategies using superconcentrated salts,concentrated diluents,polymer additives,polymer networks,and artificial passivation layers,which are used for suppressing water decomposition and widening the electrochemical stability window of water of the electrolytes.In addition,this Review discusses potential strategies for the implementation of aqueous Li-metal batteries with improved electrolyte–electrode interfaces.A comprehensive understanding of each strategy in the aqueous system will assist in the design of an aqueous electrolyte and the development of sustainable and safe high-performance batteries. 展开更多
关键词 lithium-ion battery(liB) Aqueous electrolyte Gel electrolyte Electrochemical stability window li dendrite
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Electrolyte Design for Low‑Temperature Li‑Metal Batteries:Challenges and Prospects 被引量:1
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作者 Siyu Sun Kehan Wang +3 位作者 Zhanglian Hong Mingjia Zhi Kai Zhang Jijian Xu 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第2期365-382,共18页
Electrolyte design holds the greatest opportunity for the development of batteries that are capable of sub-zero temperature operation.To get the most energy storage out of the battery at low temperatures,improvements ... Electrolyte design holds the greatest opportunity for the development of batteries that are capable of sub-zero temperature operation.To get the most energy storage out of the battery at low temperatures,improvements in electrolyte chemistry need to be coupled with optimized electrode materials and tailored electrolyte/electrode interphases.Herein,this review critically outlines electrolytes’limiting factors,including reduced ionic conductivity,large de-solvation energy,sluggish charge transfer,and slow Li-ion transportation across the electrolyte/electrode interphases,which affect the low-temperature performance of Li-metal batteries.Detailed theoretical derivations that explain the explicit influence of temperature on battery performance are presented to deepen understanding.Emerging improvement strategies from the aspects of electrolyte design and electrolyte/electrode interphase engineering are summarized and rigorously compared.Perspectives on future research are proposed to guide the ongoing exploration for better low-temperature Li-metal batteries. 展开更多
关键词 Solid electrolyte interphase li metal Low temperature Electrolyte design batteries
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Dual Additives for Stabilizing Li Deposition and SEI Formation in Anode-Free Li-Metal Batteries 被引量:1
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作者 Baolin Wu Chunguang Chen +4 位作者 Dmitri L.Danilov Zhiqiang Chen Ming Jiang Rüdiger-A.Eichel Peter H.L.Notten 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第3期84-92,共9页
Anode-free Li-metal batteries are of significant interest to energy storage industries due to their intrinsically high energy.However,the accumulative Li dendrites and dead Li continuously consume active Li during cyc... Anode-free Li-metal batteries are of significant interest to energy storage industries due to their intrinsically high energy.However,the accumulative Li dendrites and dead Li continuously consume active Li during cycling.That results in a short lifetime and low Coulombic efficiency of anode-free Li-metal batteries.Introducing effective electrolyte additives can improve the Li deposition homogeneity and solid electrolyte interphase(SEI)stability for anode-free Li-metal batteries.Herein,we reveal that introducing dual additives,composed of LiAsF6 and fluoroethylene carbonate,into a low-cost commercial carbonate electrolyte will boost the cycle life and average Coulombic efficiency of NMC‖Cu anode-free Li-metal batteries.The NMC‖Cu anode-free Li-metal batteries with the dual additives exhibit a capacity retention of about 75%after 50 cycles,much higher than those with bare electrolytes(35%).The average Coulombic efficiency of the NMC‖Cu anode-free Li-metal batteries with additives can maintain 98.3%over 100 cycles.In contrast,the average Coulombic efficiency without additives rapidly decline to 97%after only 50 cycles.In situ Raman measurements reveal that the prepared dual additives facilitate denser and smoother Li morphology during Li deposition.The dual additives significantly suppress the Li dendrite growth,enabling stable SEI formation on anode and cathode surfaces.Our results provide a broad view of developing low-cost and high-effective functional electrolytes for high-energy and long-life anode-free Li-metal batteries. 展开更多
关键词 anode-free lithium metal battery dual additives in situ Raman li growth SEI formation
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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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Boosting the cycling stability of all-solid-state lithium metal batteries through MOF-based polymeric protective layers
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作者 Hongfei Bao Diancheng Chen +9 位作者 Jiaqi Cao Pengfeng Jiang Kaili Li Runtao Liu Yuling Zhao Yichun Zheng Beiqi Liao Yaming Zhang Xia Lu Yang Sun 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期511-518,I0011,共9页
Solid-state electrolytes(SSEs)play a pivotal role in advancing next-generation lithium metal battery technology.However,they commonly encounter substantial interfacial resistance and poor stability when interfacing wi... Solid-state electrolytes(SSEs)play a pivotal role in advancing next-generation lithium metal battery technology.However,they commonly encounter substantial interfacial resistance and poor stability when interfacing with lithium metal,hindering practical applications.Herein,we introduce a flexible metal-organic framework(MOF:NUS-6)-incorporated polymeric layer,denoted as NP,designed to protect the sodium superionic conductor(NASICON)-type Li_(1.3)Al_(0.3)Ti_(1.7)(PO_(4))_(3)(LATP)electrolyte from Li metal anodes.The NP matrix establishes a soft interface with the LATP surface,effectively reducing voids and gaps that may arise between the LATP electrolyte and Li metal.Moreover,the MOF component in NP enhances ionic conductivity,offers abundant Li^(+)transport sites,and provides hierarchical ion channels,ensuring a homogeneous Li^(+)flow and thus effectively inhibiting Li dendrite formation.Utilizing NP,we fabricate Li symmetrical cells cycled for over 1600 h at 0.2 mA cm^(-2)and all-solid-state LiINP-LATPI LiFePO_(4)batteries,achieving a remarkable 99.3%capacity retention after 200 cycles at 0.2 C.This work outlines a general strategy for designing long-lasting and stable solid-state Li metal batteries. 展开更多
关键词 All-solid-state li metal battery MOF-based polymeric layer li dendrite Interfacial contact LATP electrolyte stability
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SEI/dead Li-turning capacity loss for high-performance anode-free solid-state lithium batteries
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作者 Qianwen Yin Tianyu Li +3 位作者 Hongzhang Zhang Guiming Zhong Xiaofei Yang Xianfeng Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第9期145-152,共8页
Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal batteries.However,the unclear mechanism for the fast capacity decay ... Anode-free solid-state lithium metal batteries(AF-SSLBs)have the potential to deliver higher energy density and improved safety beyond lithium-metal batteries.However,the unclear mechanism for the fast capacity decay in AF-SSLBs,either determined by dead Li or solid electrolyte interface(SEI),limits the proposal of effective strategies to prolong cycling life.To clarify the underlying mechanism,herein,the evolution of SEI and dead Li is quantitatively analyzed by a solid-state nuclear magnetic resonance(ss-NMR)technology in a typical LiPF6-based polymer electrolyte.The results show that the initial capacity loss is attributed to the formation of SEI,while the dead Li dominates the following capacity loss and the growth rate is 0.141 mA h cm^(−2)cycle−1.To reduce the active Li loss,the combination of inorganic-rich SEI and self-healing electrostatic shield effect is proposed to improve the reversibility of Li deposition/dissolution behavior,which reduces the capacity loss rate for the initial SEI and following dead Li generation by 2.3 and 20.1 folds,respectively.As a result,the initial Coulombic efficiency(ICE)and stable CE increase by 15.1%and 15.3%in Li-Cu cells,which guides the rational design of high-performance AF-SSLBs. 展开更多
关键词 Solid-state lithium batteries Solid-state NMR Anode-free SEI Dead li
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Branch-Chain-Rich Diisopropyl Ether with Steric Hindrance Facilitates Stable Cycling of Lithium Batteries at-20℃
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作者 Houzhen Li Yongchao Kang +6 位作者 Wangran Wei Chuncheng Yan Xinrui Ma Hao Chen Yuanhua Sang Hong Liu Shuhua Wang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第10期121-135,共15页
Li metal batteries(LMBs)offer signifi-cant potential as high energy density alternatives;nev-ertheless,their performance is hindered by the slow desolvation process of electrolytes,particularly at low temperatures(LT)... Li metal batteries(LMBs)offer signifi-cant potential as high energy density alternatives;nev-ertheless,their performance is hindered by the slow desolvation process of electrolytes,particularly at low temperatures(LT),leading to low coulombic efficiency and limited cycle stability.Thus,it is essential to opti-mize the solvation structure thereby achieving a rapid desolvation process in LMBs at LT.Herein,we introduce branch chain-rich diisopropyl ether(DIPE)into a 2.5 M Li bis(fluorosulfonyl)imide dipropyl ether(DPE)elec-trolyte as a co-solvent for high-performance LMBs at-20℃.The incorporation of DIPE not only enhances the disorder within the electrolyte,but also induces a steric hindrance effect form DIPE’s branch chain,excluding other solvent molecules from Li+solvation sheath.Both of these factors contribute to the weak interactions between Li^(+)and solvent molecules,effectively reducing the desolvation energy of the electrolyte.Consequently,Li(50μm)||LFP(mass loading~10 mg cm^(-2))cells in DPE/DIPE based electrolyte demonstrate stable performance over 650 cycles at-20℃,delivering 87.2 mAh g^(-1),and over 255 cycles at 25℃ with 124.8 mAh g^(-1).DIPE broadens the electrolyte design from molecular structure considera-tions,offering a promising avenue for highly stable LMBs at LT. 展开更多
关键词 Solvation structure li metal battery Low temperature Steric hindrance DISORDER
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Quantum Spin Exchange Interactions to Accelerate the Redox Kinetics in Li–S Batteries
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作者 Yu Du Weijie Chen +4 位作者 Yu Wang Yue Yu Kai Guo Gan Qu Jianan Zhang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第5期370-383,共14页
Spin-engineering with electrocatalysts have been exploited to suppress the“shuttle effect”in Li–S batteries.Spin selec-tion,spin-dependent electron mobility and spin potentials in activation barriers can be optimiz... Spin-engineering with electrocatalysts have been exploited to suppress the“shuttle effect”in Li–S batteries.Spin selec-tion,spin-dependent electron mobility and spin potentials in activation barriers can be optimized as quantum spin exchange interactions lead-ing to a significant reduction of the electronic repulsions in the orbitals of catalysts.Herein,we anchor the MgPc molecules on fluorinated carbon nanotubes(MgPc@FCNT),which exhibits the single active Mg sites with axial displacement.According to the density functional theory calculations,the electronic spin polarization in MgPc@FCNT not only increases the adsorption energy toward LiPSs intermediates but also facilitates the tunneling process of electron in Li–S batter-ies.As a result,the MgPc@FCNT provides an initial capacity of 6.1 mAh cm^(-2) even when the high sulfur loading is 4.5 mg cm^(-2),and still maintains 5.1 mAh cm^(-2) after 100 cycles.This work provides a new perspective to extend the main group single-atom catalysts enabling high-performance Li–S batteries. 展开更多
关键词 Metal phthalocyanines Spin polarization ELECTROCATALYSIS li–S batteries
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Atomistic understanding of capacity loss in LiNiO_(2)for high-nickel Li-ion batteries:First-principles study
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作者 彭率 陈丽娟 +1 位作者 何长春 杨小宝 《Chinese Physics B》 SCIE EI CAS CSCD 2024年第5期625-629,共5页
Combining the first-principles calculations and structural enumeration with recognition,the delithiation process of LiNiO_(2)is investigated,where various supercell shapes are considered in order to obtain the formati... Combining the first-principles calculations and structural enumeration with recognition,the delithiation process of LiNiO_(2)is investigated,where various supercell shapes are considered in order to obtain the formation energy of Li_(x)NiO_(2).Meanwhile,the voltage profile is simulated and the ordered phases of lithium vacancies corresponding to concentrations of 1/4,2/5,3/7,1/2,2/3,3/4,5/6,and 6/7 are predicted.To understand the capacity decay in the experiment during the charge/discharge cycles,deoxygenation and Li/Ni antisite defects are calculated,revealing that the chains of oxygen vacancies will be energetically preferrable.It can be inferred that in the absence of oxygen atom in high delithiate state,the diffusion of Ni atoms is facilitated and the formation of Li/Ni antisite is induced. 展开更多
关键词 li-ion battery ground state formation energy oxygen vacancy li/Ni antisite
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Ion-dipole regulation based on bidentate solvent for stabilizing high-voltage lithium metal batteries
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作者 Zhengyi Xu Lin Sun +4 位作者 Yang Yang Xuejia Li Yuncong Liu Xinxiu Yan Tao Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第11期432-440,共9页
The poor compatibility of ester electrolytes with lithium metal anode severely limits its use in high voltage lithium metal batteries(LMBs).In this work,a bidentate solvent 1,2-diethoxyethane(DEE) is introduced into e... The poor compatibility of ester electrolytes with lithium metal anode severely limits its use in high voltage lithium metal batteries(LMBs).In this work,a bidentate solvent 1,2-diethoxyethane(DEE) is introduced into ester electrolyte to regulate the ion-dipole interactions to enhance the solubility of LiNO_(3),which enables compatibility with Li anode and maintains the high voltage cathode stability.In the designed electrolyte,the steric effect of DEE facilitates the participation of NO_(3)^(-)and PF_6^(-)anions in the Li^(+) solvation structure,thus promoting the generation of inorganic-rich solid electrolyte interphase(SEI).And the low viscosity of DEE also ensures that the ester electrolyte poses good interracial wettability.As a result,our designed electrolyte enables the high-loading Li‖NCM622 and Li‖NCM811(^(3) mA h cm^(-2)) full cells to achieve stable cycling over 200 cycles,8 times longer than that of a conventional ester electrolyte.This work suggests that regulation of intermolecular interactions in conventional ester electrolytes is a scalable and effective approach to achieve excellent electrochemical performance of LMBs. 展开更多
关键词 Ion-dipole interactions Solvation structure Solid electrolyte interphase Ester electrolyte li metal battery
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Biphase-to-monophase structure evolution of Na_(0.766+x)Li_(x)Ni_(0.33-x)Mn_(0.5)Fe_(0.1)Ti_(0.07)O_(2) toward ultradurable Na-ion batteries
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作者 Mengting Liu Zhiwei Cheng +10 位作者 Xu Zhu Haojie Dong Tianran Yan Liang Zhang Lu Zheng Hu-Rong Yao Xian-Zuo Wang Lianzheng Yu Bing Xiao Yao Xiao Peng-Fei Wang 《Carbon Energy》 SCIE EI CAS CSCD 2024年第9期66-79,共14页
Layered composite oxide materials with O3/P2 biphasic crystallographic structure typically demonstrate a combination of high capacities of the O3 phase and high operation voltages of the P2 phase.However,their practic... Layered composite oxide materials with O3/P2 biphasic crystallographic structure typically demonstrate a combination of high capacities of the O3 phase and high operation voltages of the P2 phase.However,their practical applications are seriously obstructed by difficulties in thermodynamic phase regulation,complicated electrochemical phase transition,and unsatisfactory cycling life.Herein,we propose an efficient structural evolution strategy from biphase to monophase of Na_(0.766+x)Li_(x)Ni_(0.33-x)Mn_(0.5)Fe_(0.1)Ti_(0.07)O_(2) through Li+substitution.The role of Li+substitution not only simplifies the unfavorable phase transition by altering the local coordination of transition metal(TM)cations but also stabilizes the cathode–electrolyte interphase to prevent the degradation of TM cations during battery cycling.As a result,the thermodynamically robust O_(3)-Na_(0.826)Li_(0.06)Ni_(0.27)Mn_(0.5)Fe_(0.1)Ti_(0.07)O_(2) cathode delivers a high capacity of 139.4 mAh g^(-1) at 0.1 C and shows prolonged cycling life at high rates,with capacity retention of 81.6%at 5 C over 500 cycles.This work establishes a solid relationship between the thermodynamic structure evolution and electrochemistry of layered cathode materials,contributing to the development of long-life sodium-ion batteries. 展开更多
关键词 ELECTROCHEMISTRY li+substitution Na-ion batteries O_(3)phase phase transition
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NbN quantum dots anchored hollow carbon nanorods as efficient polysulfide immobilizer and lithium stabilizer for Li-S full batteries
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作者 Fei Ma Zhuo Chen +9 位作者 Katam Srinivas Ziheng Zhang Yu Wu Dawei Liu Hesheng Yu Yue Wang Xinsheng Li Ming-qiang Zhu Qi Wu Yuanfu Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第1期260-271,I0007,共13页
The shuttle effect of lithium polysulfides(LiPSs)and uncontrollable lithium dendrite growth seriously hinder the practical application of lithium-sulfur(Li-S)batteries.To simultaneously address such issues,monodispers... The shuttle effect of lithium polysulfides(LiPSs)and uncontrollable lithium dendrite growth seriously hinder the practical application of lithium-sulfur(Li-S)batteries.To simultaneously address such issues,monodispersed Nb N quantum dots anchored on nitrogen-doped hollow carbon nanorods(NbN@NHCR)are elaborately developed as efficient Li PSs immobilizer and Li stabilizer for high-performance Li-S full batteries.Density functional theory(DFT)calculations and experimental characterizations demonstrate that the sulfiphilic and lithiophilic NbN@NHCR hybrid can not only efficiently immobilize the soluble Li PSs and facilitate diffusion-conversion kinetics for alleviating the shuttling effect,but also homogenize the distribution of Li+ions and regulate uniform Li deposition for suppressing Li-dendrite growth.As a result,the assembled Li-S full batteries(NbN@NHCR-S||Nb N@NHCR-Li)deliver excellent long-term cycling stability with a low decay rate of 0.031%per cycle over 1000 cycles at high rate of 2 C.Even at a high S loading of 5.8 mg cm^(-2)and a low electrolyte/sulfur ratio of 5.2μL mg^(-1),a large areal capacity of 6.2 mA h cm^(-2)can be achieved in Li-S pouch cell at 0.1 C.This study provides a new perspective via designing a dual-functional sulfiphilic and lithiophilic hybrid to address serious issues of the shuttle effect of S cathode and dendrite growth of Li anode. 展开更多
关键词 Dual-functional host NbN quantum dots Shuttle effect Dendrite-free li anode li-S full batteries
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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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Structure Regulation of Electric Double Layer via Hydrogen Bonding Effect to Realize High-Stability Lithium-Metal Batteries
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作者 Sheng Liu Chaozhu Shu +8 位作者 Yu Yan Dayue Du Longfei Ren Ting Zeng Xiaojuan Wen Haoyang Xu Xinxiang Wang Guilei Tian Ying Zeng 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第3期72-83,共12页
The interfacial chemistry of solid electrolyte interphases(SEI)on lithium(Li)electrode is directly determined by the structural chemistry of the electric double layer(EDL)at the interface.Herein,a strategy for regulat... The interfacial chemistry of solid electrolyte interphases(SEI)on lithium(Li)electrode is directly determined by the structural chemistry of the electric double layer(EDL)at the interface.Herein,a strategy for regulating the structural chemistry of EDL via the introduction of intermolecular hydrogen bonds has been proposed(p-hydroxybenzoic acid(pHA)is selected as proof-of-concept).According to the molecular dynamics(MD)simulation and density functional theory(DFT)calculation results,the existence of hydrogen bonds realizes the anion structural rearrangement in the EDL,reduces the lowest unoccupied molecular orbital(LUMO)energy level of anions in the EDL,and the number of free solvent molecules,which promotes the formation of inorganic species-enriched SEI and eventually achieves the dendrite-free Li deposition.Based on this strategy,Li‖Cu cells can stably run over 185 cycles with an accumulated active Li loss of only 2.27 mAh cm^(-2),and the long-term cycle stability of Li‖Li cells is increased to 1200 h.In addition,the full cell pairing with the commercial LiFePO_(4)(LFP)cathodes exhibits stable cycling performance at 1C,with a capacity retention close to 90%after 200 cycles. 展开更多
关键词 electric double layer electrolyte additives intermolecular hydrogen bonds li metal batteries p-Hydroxybenzoic acid
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A Solvent-Free Covalent Organic Framework Single-Ion Conductor Based on Ion-Dipole Interaction for All-Solid-State Lithium Organic Batteries
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作者 Zhongping Li Kyeong-Seok Oh +6 位作者 Jeong-Min Seo Wenliang Qin Soohyoung Lee Lipeng Zhai Changqing Li Jong-Beom Baek Sang-Young Lee 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第12期189-200,共12页
Single-ion conductors based on covalent organic frameworks(COFs)have garnered attention as a potential alternative to currently prevalent inorganic ion conductors owing to their structural uniqueness and chemical vers... Single-ion conductors based on covalent organic frameworks(COFs)have garnered attention as a potential alternative to currently prevalent inorganic ion conductors owing to their structural uniqueness and chemical versatility.However,the sluggish Li+conduction has hindered their practical applications.Here,we present a class of solvent-free COF single-ion conductors(Li-COF@P)based on weak ion-dipole interaction as opposed to traditional strong ion-ion interaction.The ion(Li+from the COF)-dipole(oxygen from poly(ethylene glycol)diacrylate embedded in the COF pores)interaction in the Li-COF@P promotes ion dissociation and Li+migration via directional ionic channels.Driven by this single-ion transport behavior,the Li-COF@P enables reversible Li plating/stripping on Li-metal electrodes and stable cycling performance(88.3%after 2000 cycles)in organic batteries(Li metal anode||5,5’-dimethyl-2,2’-bis-p-benzoquinone(Me2BBQ)cathode)under ambient operating conditions,highlighting the electrochemical viability of the Li-COF@P for all-solid-state organic batteries. 展开更多
关键词 Solid organic single-ion conductors Solvent-free covalent organic frameworks All-solid-state li organic batteries Ion-dipole interaction Pore functionalization
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Sandwich-type composited solid polymer electrolytes to strengthen the interfacial ionic transportation and bulk conductivity for all-solid-state lithium batteries from room temperature to 120℃
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作者 Jiewen Tan Zhen Wang +7 位作者 Jiawu Cui Zhanhui Jia Wensheng Tian Chao Wu Chengxin Peng Chengyong Shu Kang Yang Wei Tang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期288-295,I0007,共9页
The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the m... The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the melting point,dominantly limits their applications in solid-state batteries(SSBs).Although the inorganic filler such as CeO_(2)nanoparticle content of composite solid polymer electrolytes(CSPEs)can significantly reduce the enormous charge transfer impedance at the Li metal/SPEs interface,we found that the required content of CeO_(2)nanoparticles in SPEs varies for achieving a decent interfacial charge transfer impedance and the bulk ionic conductivity in CSPEs.In this regard,a sandwich-type composited solid polymer electrolyte with a 10%CeO_(2)CSPEs interlayer sandwiched between two 50%CeO_(2)CSPEs thin layers(sandwiched CSPEs)is constructed to simultaneously achieve low charge transfer impedance and superior ionic conductivity at 30℃.The sandwiched CSPEs allow for stable cycling of Li plating and stripping for 1000 h with 129 mV polarized voltage at 0.1 mA cm^(-2)and 30℃.In addition,the LiFePO_(4)/Sandwiched CSPEs/Li cell also exhibits exceptional cycle performance at 30℃and even elevated120℃without short circuits.Constructing multi-layered CSPEs with optimized contents of the inorganic fillers can be an efficient method for developing all solid-state PEO-based batteries with high performance at a wide range of temperatures. 展开更多
关键词 PEO-based solid electrolytes CeO_(2)nanoparticles Charge transfer impedance Sandwich-type composite electrolytes All-solid-state li metal batteries
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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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All-Solid-State Thin-Film Lithium-Sulfur Batteries 被引量:8
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作者 Renming Deng Bingyuan Ke +5 位作者 Yonghui Xie Shoulin Cheng Congcong Zhang Hong Zhang Bingan Lu Xinghui Wang 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第5期326-338,共13页
Lithium-sulfur(Li-S)system coupled with thin-film solid electrolyte as a novel high-energy micro-battery has enormous potential for complementing embedded energy harvesters to enable the autonomy of the Internet of Th... Lithium-sulfur(Li-S)system coupled with thin-film solid electrolyte as a novel high-energy micro-battery has enormous potential for complementing embedded energy harvesters to enable the autonomy of the Internet of Things microdevice.However,the volatility in high vacuum and intrinsic sluggish kinetics of S hinder researchers from empirically integrating it into allsolid-state thin-film batteries,leading to inexperience in fabricating all-solid-state thin-film Li-S batteries(TFLSBs).Herein,for the first time,TFLSBs have been successfully constructed by stacking vertical graphene nanosheets-Li2S(VGsLi2S)composite thin-film cathode,lithium-phosphorous-oxynitride(LiPON)thin-film solid electrolyte,and Li metal anode.Fundamentally eliminating Lipolysulfide shuttle effect and maintaining a stable VGs-Li2S/LiPON interface upon prolonged cycles have been well identified by employing the solid-state Li-S system with an“unlimited Li”reservoir,which exhibits excellent longterm cycling stability with a capacity retention of 81%for 3,000 cycles,and an exceptional high temperature tolerance up to 60℃.More impressively,VGs-Li2S-based TFLSBs with evaporated-Li thin-film anode also demonstrate outstanding cycling performance over 500 cycles with a high Coulombic efficiency of 99.71%.Collectively,this study presents a new development strategy for secure and high-performance rechargeable all-solid-state thin-film batteries. 展开更多
关键词 All-solid-state thin-film batteries li-S batteries Vertical graphene nanosheets lithium phosphorous oxynitride li2S
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Bifunctional flame retardant solid-state electrolyte toward safe Li metal batteries 被引量:4
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作者 Qiang Lv Yajie Song +10 位作者 Bo Wang Shangjie Wang Bochen Wu Yutong Jing Huaizheng Ren Shengbo Yang Lei Wang Lihui Xiao Dianlong Wang Huakun Liu Shixue Dou 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第6期613-622,I0014,共11页
Solid polymer electrolytes(SPEs)are one of the most promising alternatives to flammable liquid electrolytes for building safe Li metal batteries.Nevertheless,the poor ionic conductivity at room temperature(RT)and low ... Solid polymer electrolytes(SPEs)are one of the most promising alternatives to flammable liquid electrolytes for building safe Li metal batteries.Nevertheless,the poor ionic conductivity at room temperature(RT)and low resistance to Li dendrites seriously hinder the commercialization of SPEs.Herein,we design a bifunctional flame retardant SPE by combining hydroxyapatite(HAP)nanomaterials with Nmethyl pyrrolidone(NMP)in the PVDF-HFP matrix.The addition of HAP generates a hydrogen bond network with the PVDF-HFP matrix and cooperates with NMP to facilitate the dissociation of Li TFSI in the PVDF-HFP matrix.Consequently,the prepared SPE demonstrates superior ionic conductivity at RT,excellent fireproof properties,and strong resistance to Li dendrites.The assembled Li symmetric cell with prepared SPE exhibits a stable cycling performance of over 1200 h at 0.2 m A cm^(-2),and the solid-state LiFePO_4||Li cell shows excellent capacity retention of 85.3%over 600 cycles at 0.5 C. 展开更多
关键词 Solid polymer electrolytes Safe li metal batteries li dendrites Hydroxyapatite N-methyl pyrrolidone PVDF-HFP Fireproof property
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Rational Design of High-Performance PEO/Ceramic Composite Solid Electrolytes for Lithium Metal Batteries 被引量:6
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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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