All-solid-state batteries(ASSBs)have garnered significant interest as the next-generation in battery technology,praised for their superior safety and high energy density.However,a conductive agent accelerates the unde...All-solid-state batteries(ASSBs)have garnered significant interest as the next-generation in battery technology,praised for their superior safety and high energy density.However,a conductive agent accelerates the undesirable side reactions of sulfide-based solid electrolytes(SEs),resulting in poor electrochemical properties with increased interfacial resistance.Here,we propose a wet chemical method rationally designed to achieve a conformal coating of lithium-indium chloride(Li_(3)InCl_(6))onto vapor-grown carbon fibers(VGCFs)as conductive agents.First,with the advantage of the Li_(3)InCl_(6) protective layer,use of VGCF@Li_(3)InCl_(6) leads to enhanced interfacial stability and improved electrochemical properties,including stable cycle performance.These results indicate that the Li_(3)InCl_(6) protective layer suppresses the unwanted reaction between Li_(6)PS_(5)Cl(LPSCl)and VGCF.Second,VGCF@Li_(3)InCl_(6) effectively promotes polytetrafluoroethylene(PTFE)fibrillization,leading to a homogeneous electrode microstructure.The uniform distribution of the cathode active material(CAM)in the electrode results in reduced charge-transfer resistance(R_(ct))and enhanced Li-ion kinetics.As a result,a full cell with the LiNi_(x)Mn_(y)Co_(z)O_(2)(NCM)/VGCF@Li_(3)InCl_(6) electrode shows an areal capacity of 7.7mAhcm^(−2) at 0.05 C and long-term cycle stability of 77.9%over 400 cycles at 0.2 C.This study offers a strategy for utilizing stable carbon-based conductive agents in sulfide-based ASSBs to enhance their electrochemical performance.展开更多
Anode-free all-solid-state batteries(AF-ASSBs)have received significant attention as a next-generation battery system due to their high energy density and safety.However,this system still faces challenges,such as poor...Anode-free all-solid-state batteries(AF-ASSBs)have received significant attention as a next-generation battery system due to their high energy density and safety.However,this system still faces challenges,such as poor Coulombic efficiency and short-circuiting caused by Li dendrite growth.In this study,the AF-ASSBs are demonstrated with reliable and robust electrochemical properties by employing Cu-Sn nanotube(NT)thin layer(~1μm)on the Cu current collector for regulating Li electrodeposition.Li_(x)Sn phases with high Li-ion diffusivity in the lithiated Cu-Sn NT layer enable facile Li diffusion along with its one-dimensional hollow geometry.The unique structure,in which Li electrodeposition takes place between the Cu-Sn NT layer and the current collector by the Coble creep mechanism,improves cell durability by preventing solid electrolyte(SE)decomposition and Li dendrite growth.Furthermore,the large surface area of the Cu-Sn NT layer ensures close contact with the SE layer,leading to a reduced lithiation overpotential compared to that of a flat Cu-Sn layer.The Cu-Sn NT layer also maintains its structural integrity owing to its high mechanical properties and porous nature,which could further alleviate the mechanical stress.The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM)|SE|Cu-Sn NT@Cu cell with a practical capacity of 2.9 mAh cm^(−2) exhibits 83.8%cycle retention after 150 cycles and an average Coulombic efficiency of 99.85%at room temperature.It also demonstrates a critical current density 4.5 times higher compared to the NCM|SE|Cu cell.展开更多
EPW is an open-source software for ab initio calculations of electron–phonon interactions and related materials properties.The code combines density functional perturbation theory and maximally localized Wannier func...EPW is an open-source software for ab initio calculations of electron–phonon interactions and related materials properties.The code combines density functional perturbation theory and maximally localized Wannier functions to efficiently compute electron–phonon coupling matrix elements,and to perform predictive calculations of temperature-dependent properties and phonon-assisted quantum processes in bulk solids and low-dimensional materials.Here,we report on significant developments in the code since 2016,namely:a transport module for the calculation of charge carrier mobility under electric and magnetic fields using the Boltzmann transport equation;a superconductivity module for calculations of phonon-mediated superconductors using the anisotropic multi-band Eliashberg theory;an optics module for calculations of phonon-assisted indirect transitions;a module for the calculation of small and large polarons without supercells;and a module for calculating band structure renormalization and temperature-dependent optical spectra using the special displacement method.For each capability,we outline the methodology and implementation and provide example calculations.展开更多
基金supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korean Government(MOTIE)(RS-2024-00417730,HRD Program for Industrial Innovation)supported by the Technology Innovation Program(or Industrial Strategic Technology Development Program-Materials&Components Technology Development Program)(20024261),Development of thick film electrodes and cell manufacturing technology for a high-performance lithium iron phosphate battery with energy density of over 200 Wh/kg was funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea).
文摘All-solid-state batteries(ASSBs)have garnered significant interest as the next-generation in battery technology,praised for their superior safety and high energy density.However,a conductive agent accelerates the undesirable side reactions of sulfide-based solid electrolytes(SEs),resulting in poor electrochemical properties with increased interfacial resistance.Here,we propose a wet chemical method rationally designed to achieve a conformal coating of lithium-indium chloride(Li_(3)InCl_(6))onto vapor-grown carbon fibers(VGCFs)as conductive agents.First,with the advantage of the Li_(3)InCl_(6) protective layer,use of VGCF@Li_(3)InCl_(6) leads to enhanced interfacial stability and improved electrochemical properties,including stable cycle performance.These results indicate that the Li_(3)InCl_(6) protective layer suppresses the unwanted reaction between Li_(6)PS_(5)Cl(LPSCl)and VGCF.Second,VGCF@Li_(3)InCl_(6) effectively promotes polytetrafluoroethylene(PTFE)fibrillization,leading to a homogeneous electrode microstructure.The uniform distribution of the cathode active material(CAM)in the electrode results in reduced charge-transfer resistance(R_(ct))and enhanced Li-ion kinetics.As a result,a full cell with the LiNi_(x)Mn_(y)Co_(z)O_(2)(NCM)/VGCF@Li_(3)InCl_(6) electrode shows an areal capacity of 7.7mAhcm^(−2) at 0.05 C and long-term cycle stability of 77.9%over 400 cycles at 0.2 C.This study offers a strategy for utilizing stable carbon-based conductive agents in sulfide-based ASSBs to enhance their electrochemical performance.
基金Korea Institute of Energy Technology Evaluation and Planning,Grant/Award Number:20214000000520Ministry of Trade,Industry and Energy,Grant/Award Number:20009985。
文摘Anode-free all-solid-state batteries(AF-ASSBs)have received significant attention as a next-generation battery system due to their high energy density and safety.However,this system still faces challenges,such as poor Coulombic efficiency and short-circuiting caused by Li dendrite growth.In this study,the AF-ASSBs are demonstrated with reliable and robust electrochemical properties by employing Cu-Sn nanotube(NT)thin layer(~1μm)on the Cu current collector for regulating Li electrodeposition.Li_(x)Sn phases with high Li-ion diffusivity in the lithiated Cu-Sn NT layer enable facile Li diffusion along with its one-dimensional hollow geometry.The unique structure,in which Li electrodeposition takes place between the Cu-Sn NT layer and the current collector by the Coble creep mechanism,improves cell durability by preventing solid electrolyte(SE)decomposition and Li dendrite growth.Furthermore,the large surface area of the Cu-Sn NT layer ensures close contact with the SE layer,leading to a reduced lithiation overpotential compared to that of a flat Cu-Sn layer.The Cu-Sn NT layer also maintains its structural integrity owing to its high mechanical properties and porous nature,which could further alleviate the mechanical stress.The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM)|SE|Cu-Sn NT@Cu cell with a practical capacity of 2.9 mAh cm^(−2) exhibits 83.8%cycle retention after 150 cycles and an average Coulombic efficiency of 99.85%at room temperature.It also demonstrates a critical current density 4.5 times higher compared to the NCM|SE|Cu cell.
基金This research is supported by:the Computational Materials Sciences Program funded by the U.S.Department of Energy,Office of Science,Basic Energy Sciences,under Award No.DE-SC0020129(project coordination,scale-up,polaron module,transport module,optics module,special displacement module)the National Science Foundation,Office of Advanced Cyberinfrastructure and Division of Materials Research under Grants Nos.2103991 and 2035518(superconductivity module,interoperability)+12 种基金the NSF Characteristic Science Applications for the Leadership Class Computing Facility program under Grant No.2139536(prepara-tion for LCCF)the Fond National de la Recherche Scientifique of Belgium(F.R.S.-FNRS)and the European Union’s Horizon 2020 research and innovation program under grant agreements No.881603-Graphene Core3(transport module)the NSF DMREF award 2119555(quasi-degenerate perturbation theory module)This research used resources of the National Energy Research Scientific Computing Center and the Argonne Leadership Computing Facility,which are DOE Office of Science User Facilities supported by the Office of Science of the U.S.Department of Energy,under Contracts No.DE-AC02-05CH11231 and DE-AC02-06CH11357,respectivelyThe authors acknowledge the Texas Advanced Computing Center(TACC)at The University of Texas at Austin for providing access to Frontera,Lonestar6,and Texascale Days,which have contributed to the research results reported within this paper(http://www.tacc.utexas.edu)the Extreme Science and Engineering Discovery Environment(XSEDE)218 which is supported by National Science Foundation grant number ACI-1548562in particular Expanse at the San Diego Supercomputer Center through allocation TG-DMR180071.S.Packnowl-edges computational resources provided by the PRACE award granting access to Discoverer in SofiaTech,Bulgaria(OptoSpin project id.2020225411)by the Consortium desÉquipements de Calcul Intensif(CÉCI),funded by the FRS-FNRS under Grant No.2.5020.11the Walloon Region,as well as computational resources awarded on the Belgian share of the EuroHPC LUMI supercomputer.K.B.acknowledges the support of the U.S.Department of Energy,Office of Science,Office of Advanced Scientific Computing Research,Department of Energy Computational Science Graduate Fellowship under Award Number DE-SC0020347The authors wish to thank Zhenbang Dai,Nikolaus Kandolf,Viet-Anh Ha,and Amanda Wang for their contributions to the EPW project that are not discussed in this manuscriptJohn Cazes and Hang Liu at TACC for their support with the Characteristic Science Applications project,Paolo Giannozzi for his support with Quantum ESPRESSOStefano Baroni for fruitful discussions.
文摘EPW is an open-source software for ab initio calculations of electron–phonon interactions and related materials properties.The code combines density functional perturbation theory and maximally localized Wannier functions to efficiently compute electron–phonon coupling matrix elements,and to perform predictive calculations of temperature-dependent properties and phonon-assisted quantum processes in bulk solids and low-dimensional materials.Here,we report on significant developments in the code since 2016,namely:a transport module for the calculation of charge carrier mobility under electric and magnetic fields using the Boltzmann transport equation;a superconductivity module for calculations of phonon-mediated superconductors using the anisotropic multi-band Eliashberg theory;an optics module for calculations of phonon-assisted indirect transitions;a module for the calculation of small and large polarons without supercells;and a module for calculating band structure renormalization and temperature-dependent optical spectra using the special displacement method.For each capability,we outline the methodology and implementation and provide example calculations.
