Fluoropolymers promise all-solid-state lithium metal batteries(ASLMBs)but suffer from two critical challenges.The first is the trade-off between ionic conductivity(σ)and lithium anode reactions,closely related to hig...Fluoropolymers promise all-solid-state lithium metal batteries(ASLMBs)but suffer from two critical challenges.The first is the trade-off between ionic conductivity(σ)and lithium anode reactions,closely related to high-content residual solvents.The second,usually consciously overlooked,is the fluoropolymer's inherent instability against alkaline lithium anodes.Here,we propose indium-based metal-organic frameworks(In-MOFs)as a multifunctional promoter to simultaneously address these two challenges,using poly(vinylidene fluoride-hexafluoropropylene)(PVH)as the typical fluoropolymer.In-MOF plays a trio:(1)adsorbing and converting free residual solvents into bonded states to prevent their side reactions with lithium anodes while retaining their advantages on Li~+transport;(2)forming inorganic-rich solid electrolyte interphase layers to prevent PVH from reacting with lithium anodes and promote uniform lithium deposition without dendrite growth;(3)reducing PVH crystallinity and promoting Li-salt dissociation.Therefore,the resulting PVH/In-MOF(PVH-IM)showcases excellent electrochemical stability against lithium anodes,delivering a 5550 h cycling at 0.2 m A cm^(-2)with a remarkable cumulative lithium deposition capacity of 1110 m Ah cm^(-2).It also exhibits an ultrahighσof 1.23×10^(-3)S cm^(-1)at 25℃.Moreover,all-solid-state LiFePO_4|PVH-IM|Li full cells show outstanding rate capability and cyclability(80.0%capacity retention after 280 cycles at 0.5C),demonstrating high potential for practical ASLMBs.展开更多
For future clean energy demand,it is essential to develop highly efficient and durable materials for use in renewable energy conversion devices.Herein,we report an electrocatalyst loaded with Pd-Pb-Bi nanoalloys on re...For future clean energy demand,it is essential to develop highly efficient and durable materials for use in renewable energy conversion devices.Herein,we report an electrocatalyst loaded with Pd-Pb-Bi nanoalloys on reduced graphene(rGO)-wrapped In_(2)O_(3)(PdPbBi@rGO/In_(2)O_(3))prepared by a hydrothermal method.PdPbBi@rGO/In_(2)O_(3)exhibits higher forward current density(229.12 mA·cm^(-2)),larger electrochemical active surface area(ECSA)(85.87 m^(2)·g^(-1)Pd),smaller impedance(12.68Ω)and lower E_(onset)(-0.56 V)than commercial Pd/C.Specifically,the current density and ECS A are 8.46 and3.38 times higher than those of commercial Pd/C(27.07 mA·cm^(-2),25.41 m^(2)·g^(-1)Pd),respectively.Furthermore,the oxidation mechanism of ethylene glycol and the removal of carbon monoxide[CO]_(ads)from the surface of Pd are also discussed in detail.The columnar support structure wrapped by rGO provides a huge active surface area for catalysis.Moreover,the electronic effect of Pd-PbBi nanoalloys can accelerate the removal of CO intermediate species,obtain more Pd active sites and improve the electrocatalytic performance.Our first synthesis of this highly electrocatalyst offers promising value for commercial application in direct fuel cells.展开更多
基金the financial support from the 261 Project of MIITNatural Science Foundation of Jiangsu Province(No.BK20240179)。
文摘Fluoropolymers promise all-solid-state lithium metal batteries(ASLMBs)but suffer from two critical challenges.The first is the trade-off between ionic conductivity(σ)and lithium anode reactions,closely related to high-content residual solvents.The second,usually consciously overlooked,is the fluoropolymer's inherent instability against alkaline lithium anodes.Here,we propose indium-based metal-organic frameworks(In-MOFs)as a multifunctional promoter to simultaneously address these two challenges,using poly(vinylidene fluoride-hexafluoropropylene)(PVH)as the typical fluoropolymer.In-MOF plays a trio:(1)adsorbing and converting free residual solvents into bonded states to prevent their side reactions with lithium anodes while retaining their advantages on Li~+transport;(2)forming inorganic-rich solid electrolyte interphase layers to prevent PVH from reacting with lithium anodes and promote uniform lithium deposition without dendrite growth;(3)reducing PVH crystallinity and promoting Li-salt dissociation.Therefore,the resulting PVH/In-MOF(PVH-IM)showcases excellent electrochemical stability against lithium anodes,delivering a 5550 h cycling at 0.2 m A cm^(-2)with a remarkable cumulative lithium deposition capacity of 1110 m Ah cm^(-2).It also exhibits an ultrahighσof 1.23×10^(-3)S cm^(-1)at 25℃.Moreover,all-solid-state LiFePO_4|PVH-IM|Li full cells show outstanding rate capability and cyclability(80.0%capacity retention after 280 cycles at 0.5C),demonstrating high potential for practical ASLMBs.
基金financially supported by the Key Laboratory of Organic Functional Molecule Synthesis and Applications,Ministry of Education(No.KLSAOFM1913)。
文摘For future clean energy demand,it is essential to develop highly efficient and durable materials for use in renewable energy conversion devices.Herein,we report an electrocatalyst loaded with Pd-Pb-Bi nanoalloys on reduced graphene(rGO)-wrapped In_(2)O_(3)(PdPbBi@rGO/In_(2)O_(3))prepared by a hydrothermal method.PdPbBi@rGO/In_(2)O_(3)exhibits higher forward current density(229.12 mA·cm^(-2)),larger electrochemical active surface area(ECSA)(85.87 m^(2)·g^(-1)Pd),smaller impedance(12.68Ω)and lower E_(onset)(-0.56 V)than commercial Pd/C.Specifically,the current density and ECS A are 8.46 and3.38 times higher than those of commercial Pd/C(27.07 mA·cm^(-2),25.41 m^(2)·g^(-1)Pd),respectively.Furthermore,the oxidation mechanism of ethylene glycol and the removal of carbon monoxide[CO]_(ads)from the surface of Pd are also discussed in detail.The columnar support structure wrapped by rGO provides a huge active surface area for catalysis.Moreover,the electronic effect of Pd-PbBi nanoalloys can accelerate the removal of CO intermediate species,obtain more Pd active sites and improve the electrocatalytic performance.Our first synthesis of this highly electrocatalyst offers promising value for commercial application in direct fuel cells.
