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Trend of Developing Aqueous Liquid and Gel Electrolytes for Sustainable,Safe,and High‑Performance Li‑Ion Batteries 被引量:1
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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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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 lis batteries
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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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Electrolyte Design for Low‑Temperature Li‑Metal Batteries:Challenges and Prospects
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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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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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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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Configuring single-layer MXene nanosheet onto natural wood fiber via C-Ti-C covalent bonds for high-stability Li-S batteries
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作者 Yangyang Chen Yu Liao +5 位作者 Ying Wu Lei Li Zhen Zhang Sha Luo Yiqiang Wu Yan Qing 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期701-711,I0016,共12页
Lithium-sulfur batteries(LSBs)are considered promising candidates for next-generation battery technologies owing to their outstanding theoretical energy density and cost-effectiveness.However,the low conductivity and ... Lithium-sulfur batteries(LSBs)are considered promising candidates for next-generation battery technologies owing to their outstanding theoretical energy density and cost-effectiveness.However,the low conductivity and polysulfide shuttling effect of S cathodes severely hamper the practical performance of LSBs.Herein,in situ-generated single layer MXene nanosheet/hierarchical porous carbonized wood fiber(MX/PCWF)composites are prepared via a nonhazardous eutectic activation strategy coupled with pyrolysis-induced gas diffusion.The unique architecture,wherein single layer MXene nanosheets are constructed on carbonized wood fiber walls,ensures rapid polysulfide conversion and continuous electron transfer for redox reactions.The C-Ti-C bonds formed between MXene and PCWF can considerably expedite the conversion of polysulfides,effectively suppressing the shuttle effect.An impressive capacity of 1301.1 m A h g^(-1)at 0.5 C accompanied by remarkable stability is attained with the MX/PCWF host,as evidenced by the capacity maintenance of 722.6 m A h g^(-1)after 500 cycles.Notably,the MX/PCWF/S cathode can still deliver a high capacity of 886.8 m A h g^(-1)at a high S loading of 5.6 mg cm^(-2).The construction of two-dimensional MXenes on natural wood fiber walls offers a competitive edge over S-based cathode materials and demonstrates a novel strategy for developing high-performance batteries. 展开更多
关键词 lithium-sulfur batteries s cathodes MXene nanosheets Wood fiber C-Ti-C bonds
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Thin polymer electrolyte with MXene functional layer for uniform Li^(+) deposition in all-solid-state lithium battery
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作者 Weijie Kou Yafang Zhang +3 位作者 Wenjia Wu Zibiao Guo Quanxian Hua Jingtao Wang 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第1期71-80,共10页
Solid polymer electrolyte(SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility;however, the unfavourable Li+deposition and large thickness hamper its development and ... Solid polymer electrolyte(SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility;however, the unfavourable Li+deposition and large thickness hamper its development and application. Herein, a laminar MXene functional layer-thin SPE layer-cathode integration(MXene-PEO-LFP) is designed and fabricated. The MXene functional layer formed by stacking rigid MXene nanosheets imparts higher compressive strength relative to PEO electrolyte layer. And the abundant negatively-charged groups on MXene functional layer effectively repel anions and attract cations to adjust the charge distribution behavior at electrolyte–anode interface. Furthermore,the functional layer with rich lithiophilic groups and outstanding electronic conductivity results in low Li nucleation overpotential and nucleation energy barrier. In consequence, the cell assembled with MXene-PEO-LFP, where the PEO electrolyte layer is only 12 μm, much thinner than most solid electrolytes, exhibits uniform, dendrite-free Li+deposition and excellent cycling stability. High capacity(142.8 mAh g-1), stable operation of 140 cycles(capacity decay per cycle, 0.065%), and low polarization potential(0.5 C) are obtained in this Li|MXene-PEO-LFP cell,which is superior to most PEO-based electrolytes under identical condition. This integrated design may provide a strategy for the large-scale application of thin polymer electrolytes in all-solid-state battery. 展开更多
关键词 MXene nanosheet Laminar functional layer Thin polymer electrolyte Dendrite-free liþdeposition All-solid-state lithium battery
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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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Accelerating lithium-sulfur battery reaction kinetics and inducing 3D deposition of Li_(2)S using interactions between Fe_(3)Se_(4)and lithium polysulfides
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作者 Yihan Lin Liheng Li +5 位作者 Longjie Tan Yongliang Li Xiangzhong Ren Peixin Zhang Chuanxin He Lingna Sun 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期540-553,I0012,共15页
Although lithium-sulfur batteries(LSBs)exhibit high theoretical energy density,their practical application is hindered by poor conductivity of the sulfur cathode,the shuttle effect,and the irreversible deposition of L... Although lithium-sulfur batteries(LSBs)exhibit high theoretical energy density,their practical application is hindered by poor conductivity of the sulfur cathode,the shuttle effect,and the irreversible deposition of Li_(2)S.To address these issues,a novel composite,using electrospinning technology,consisting of Fe_(3)Se_(4)and porous nitrogen-doped carbon nanofibers was designed for the interlayer of LSBs.The porous carbon nanofiber structure facilitates the transport of ions and electrons,while the Fe_(3)Se_(4)material adsorbs lithium polysulfides(LiPSs)and accelerates its catalytic conversion process.Furthermore,the Fe_(3)Se_(4)material interacts with soluble LiPSs to generate a new polysulfide intermediate,Li_(x)FeS_(y)complex,which changes the electrochemical reaction pathway and facilitates the three-dimensional deposition of Li_(2)S,enhancing the reversibility of LSBs.The designed LSB demonstrates a high specific capacity of1529.6 mA h g^(-1)in the first cycle at 0.2 C.The rate performance is also excellent,maintaining an ultra-high specific capacity of 779.7 mA h g^(-1)at a high rate of 8 C.This investigation explores the mechanism of the interaction between the interlayer and LiPSs,and provides a new strategy to regulate the reaction kinetics and Li_(2)S deposition in LSBs. 展开更多
关键词 lithium-sulfur batteries Polysulfide intermediates li_(2)s electrodeposition INTERLAYERs Electrostatic spinning Adsorption Catalysis
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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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Lithium-Ion Charged Polymer Channels Flattening Lithium Metal Anode 被引量:1
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作者 Haofan Duan Yu You +11 位作者 Gang Wang Xiangze Ou Jin Wen Qiao Huang Pengbo Lyu Yaru Liang Qingyu Li Jianyu Huang Yun‑Xiao Wang Hua‑Kun Liu Shi Xue Dou Wei‑Hong Lai 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第4期379-393,共15页
The concentration difference in the near-surface region of lithium metal is the main cause of lithium dendrite growth.Resolving this issue will be key to achieving high-performance lithium metal batteries(LMBs).Herein... The concentration difference in the near-surface region of lithium metal is the main cause of lithium dendrite growth.Resolving this issue will be key to achieving high-performance lithium metal batteries(LMBs).Herein,we construct a lithium nitrate(LiNO_(3))-implanted electroactiveβphase polyvinylidene fluoride-co-hexafluoropropylene(PVDF-HFP)crystalline polymorph layer(PHL).The electronegatively charged polymer chains attain lithium ions on the surface to form lithium-ion charged channels.These channels act as reservoirs to sustainably release Li ions to recompense the ionic flux of electrolytes,decreasing the growth of lithium dendrites.The stretched molecular channels can also accelerate the transport of Li ions.The combined effects enable a high Coulombic efficiency of 97.0%for 250 cycles in lithium(Li)||copper(Cu)cell and a stable symmetric plating/stripping behavior over 2000 h at 3 mA cm^(-2)with ultrahigh Li utilization of 50%.Furthermore,the full cell coupled with PHL-Cu@Li anode and Li Fe PO_(4) cathode exhibits long-term cycle stability with high-capacity retention of 95.9%after 900 cycles.Impressively,the full cell paired with LiNi_(0.87)Co_(0.1)Mn_(0.03)O_(2)maintains a discharge capacity of 170.0 mAh g^(-1)with a capacity retention of 84.3%after 100 cycles even under harsh condition of ultralow N/P ratio of 0.83.This facile strategy will widen the potential application of LiNO_(3)in ester-based electrolyte for practical high-voltage LMBs. 展开更多
关键词 Polymer ionic channel li metal batteries Artificial protective layer Uniform li deposition Electrochemical performances
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对二维Graphene/VS_(2)/BN范德华多层异质结构作为LIBs的阳极材料的相关研究
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作者 伍虎 唐贵平 +1 位作者 肖事成 范志强 《电子学报》 EI CAS CSCD 北大核心 2024年第5期1543-1552,共10页
通过范德华尔斯作用将单层石墨烯(Graphene)、单层二硫化钒(VS2)和单层氮化硼(BN)构建成Graphene/VS2/BN范德华三层异质结构,并将其与不同数量的锂结合,研究了其作为锂离子电池(Li-Ion Batterys,LIBs)中阳极电极材料的可行性.Graphene/V... 通过范德华尔斯作用将单层石墨烯(Graphene)、单层二硫化钒(VS2)和单层氮化硼(BN)构建成Graphene/VS2/BN范德华三层异质结构,并将其与不同数量的锂结合,研究了其作为锂离子电池(Li-Ion Batterys,LIBs)中阳极电极材料的可行性.Graphene/VS_(2)/BN范德华三层异质结构具有-0.33 e V/A2的形成能,具有较强的稳定性,理论上可实现合成.同时,计算了Graphene/VS_(2)/BN范德华异质结构的平面内刚度,得出的杨氏模量(Y)为886.88 N/m,高于单层VS_(2)的Y(82.5 N/m),具有较好的力学性能.Graphene/VS_(2)/BN范德华三层异质结构表面和界面上吸附Li的吸附能(-5~-2 e V)远大于相应单层的吸附能,表明其对Li具有较好的吸附性能.Li在Graphene/VS_(2)/BN范德华三层异质结构的不同表面和界面处迁移时的扩散势垒非常小(0.3~0.6 e V),对电池速率性能极为有利.Graphene/VS_(2)/BN范德华三层异质结构在LIBs的阳极电极材料方面的应用具有广泛的前景. 展开更多
关键词 石墨烯 异质结 吸附能 开路电压 能带 锂离子电池
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All-Solid-State Thin-Film Lithium-Sulfur Batteries 被引量:4
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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:3
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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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Boosting Lean Electrolyte Lithium-Sulfur Battery Performance with Transition Metals: A Comprehensive Review 被引量:2
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作者 Hui Pan Zhibin Cheng +8 位作者 Zhenyu Zhou Sijie Xie Wei Zhang Ning Han Wei Guo Jan Fransaer Jiangshui Luo Andreu Cabot Michael Wübbenhorst 《Nano-Micro Letters》 SCIE EI CAS CSCD 2023年第10期53-100,共48页
Lithium–sulfur(Li–S) batteries have received widespread attention, and lean electrolyte Li–S batteries have attracted additional interest because of their higher energy densities. This review systematically analyze... Lithium–sulfur(Li–S) batteries have received widespread attention, and lean electrolyte Li–S batteries have attracted additional interest because of their higher energy densities. This review systematically analyzes the effect of the electrolyte-to-sulfur(E/S) ratios on battery energy density and the challenges for sulfur reduction reactions(SRR) under lean electrolyte conditions. Accordingly, we review the use of various polar transition metal sulfur hosts as corresponding solutions to facilitate SRR kinetics at low E/S ratios(< 10 μL mg~(-1)), and the strengths and limitations of different transition metal compounds are presented and discussed from a fundamental perspective. Subsequently, three promising strategies for sulfur hosts that act as anchors and catalysts are proposed to boost lean electrolyte Li–S battery performance. Finally, an outlook is provided to guide future research on high energy density Li–S batteries. 展开更多
关键词 Transition metals Lean electrolyte sulfur reduction reactions lis batteries
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Li intercalation in an MoSe_(2) electrocatalyst:In situ observation and modulation of its precisely controllable phase engineering for a high-performance flexible Li-S battery 被引量:3
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作者 Yunke Wang Yige Zhao +5 位作者 Kangli Liu Shaobin Wang Neng Li Guosheng Shao Feng Wang Peng Zhang 《Carbon Energy》 SCIE CSCD 2023年第2期201-215,共15页
Sophisticated efficient electrocatalysts are essential to rectifying the shuttle effect and realizing the high performance of flexible lithium-sulfur batteries(LSBs).Phase transformation of MoSe_(2) from the 2H phase ... Sophisticated efficient electrocatalysts are essential to rectifying the shuttle effect and realizing the high performance of flexible lithium-sulfur batteries(LSBs).Phase transformation of MoSe_(2) from the 2H phase to the 1T phase has been proven to be a significant method to improve the catalytic activity.However,precisely controllable phase engineering of MoSe_(2) has rarely been reported.Herein,by in situ Li ions intercalation in MoSe_(2),a precisely controllable phase evolution from 2H-MoSe_(2) to 1T-MoSe_(2) was realized.More importantly,the definite functional relationship between cut-off voltage and phase structure was first identified for phase engineering through in situ observation and modulation methods.The sulfur host(CNFs/1T-MoSe_(2))presents high charge density,strong polysulfides adsorption,and catalytic kinetics.Moreover,Li-S cells based on it display capacity retention of 875.3mAh g^(-1) after 500 cycles at 1 C and an areal capacity of 8.71mAh cm^(-2) even at a high sulfur loading of 8.47mg cm^(-2).Furthermore,the flexible pouch cell exhibiting decent performance will endow a promising potential in the wearable energy storage field.This study proposes an effective strategy to precisely control the phase structure of MoSe_(2),which may provide the reference to fabricate the highly efficient electrocatalysts for LSBs and other energy systems. 展开更多
关键词 ELECTROCATALYsTs ELECTROsPINNING li intercalation lithium-sulfur batteries phase engineering
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