Anode-free lithium-metal batteries(AFLMBs)offer high energy density.However,lithium dendrite growth and interfacial instability remain critical obstacles to their commercialization.Here,lithiophilic nanosized(∼5 nm)L...Anode-free lithium-metal batteries(AFLMBs)offer high energy density.However,lithium dendrite growth and interfacial instability remain critical obstacles to their commercialization.Here,lithiophilic nanosized(∼5 nm)LixSn combined with an inorganic-rich@polymer dual-layer structure was constructed on a Cu current collector,prepared via a galvanostatic process using a dual-lithium salt electrolyte in a Cu||Cu configuration.The polymer outer layer,initiated by LixSn,reinforces the solid electrolyte interphase(SEI),providing mechanical robustness and enabling stable cycling in an ether-based electrolyte.Furthermore,the Sn and LixSn particle sizes can be effectively tuned by adjusting the galvanostatic discharge current.The nanosized LixSn significantly lowers the nucleation overpotential and creates abundant lithiophilic nucleation sites,resulting in uniform,dense Li plating/stripping.The modified Cu collector demonstrates superior performance in ether-based electrolytes,achieving over 92%capacity retention after 100 cycles at a current density of 1.5 mA cm^(−2)and an area capacity of 1.1 mAh cm^(−2).This work provides a simple,eco-friendly,and scalable approach for fabricating high-performance anode-free current collectors for AFLMBs.展开更多
As a noble metal substitute,two-dimensional(2D)hierarchical nano-frame structures have attracted great interest as candidate catalysts due to their remarkable advantages-high intrinsic activity,high electron mobility,...As a noble metal substitute,two-dimensional(2D)hierarchical nano-frame structures have attracted great interest as candidate catalysts due to their remarkable advantages-high intrinsic activity,high electron mobility,and straightforward surface functionalization.Therefore,they may replace Pt-based catalysts in oxygen reduction reaction(ORR)applications.Herein,a simple method is developed to design hierarchical nano-frame structures assembled via 2D NiO and N-doped graphene(NG)nanosheets.This procedure can yield nanostructures that satisfy the criteria correlated with improved electrocatalytic performance,such as large surface area,numerous undercoordinated atoms,and high defect densities.Further,porous NG nanosheet architectures,featuring NiO nanosheets densely coordinated with accessible holey Fe_(2)O_(3) moieties,can enhance mesoporosity and balance hydrophilicity.Such improvements can facilitate charge transport and expose formerly inaccessible reaction sites,maximizing active site density utilization.Density functional theory(DFT)calculations reveal favored O_(2) adsorption and dissociation on Fe_(2)O_(3) hybrid structures when supported by 2D NiO and NG nanomaterials,given 2D materials donated charge to Fe_(2)O_(3) active sites.Our systematic studies reveal that synergistic contributions are responsible for enriching the catalytic activity of Fe_(2)O_(3)@NiO/NG in alkaline media-encompassing internal voids and pores,unique hierarchical support structures,and concentrated N-dopant and bimetallic atomic interactions.Ultimately,this work expands the toolbox for designing and synthesizing highly efficient 2D/2D shelled functional nanomaterials with transition metals,endeavoring to benefit energy conversion and related ORR applications.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean Government(MSIT)(No.2020R1A5A1019131)This work was supported by a Korea Institute of Energy Technology Evaluation and Planning(KETEP)grant funded by the Korean government(MOTIE)(RS-2022-KP002703,Sector coupling energy industry advancement manpower training program)This work was supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)and the Ministry of Trade,Industry&Energy(MOTlE)of the Republic of Korea(RS-2024-00469587).
文摘Anode-free lithium-metal batteries(AFLMBs)offer high energy density.However,lithium dendrite growth and interfacial instability remain critical obstacles to their commercialization.Here,lithiophilic nanosized(∼5 nm)LixSn combined with an inorganic-rich@polymer dual-layer structure was constructed on a Cu current collector,prepared via a galvanostatic process using a dual-lithium salt electrolyte in a Cu||Cu configuration.The polymer outer layer,initiated by LixSn,reinforces the solid electrolyte interphase(SEI),providing mechanical robustness and enabling stable cycling in an ether-based electrolyte.Furthermore,the Sn and LixSn particle sizes can be effectively tuned by adjusting the galvanostatic discharge current.The nanosized LixSn significantly lowers the nucleation overpotential and creates abundant lithiophilic nucleation sites,resulting in uniform,dense Li plating/stripping.The modified Cu collector demonstrates superior performance in ether-based electrolytes,achieving over 92%capacity retention after 100 cycles at a current density of 1.5 mA cm^(−2)and an area capacity of 1.1 mAh cm^(−2).This work provides a simple,eco-friendly,and scalable approach for fabricating high-performance anode-free current collectors for AFLMBs.
基金supported by the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(MSIT)(RS2023-00235596)and ERC Center(2022R1A5A1033719)。
文摘As a noble metal substitute,two-dimensional(2D)hierarchical nano-frame structures have attracted great interest as candidate catalysts due to their remarkable advantages-high intrinsic activity,high electron mobility,and straightforward surface functionalization.Therefore,they may replace Pt-based catalysts in oxygen reduction reaction(ORR)applications.Herein,a simple method is developed to design hierarchical nano-frame structures assembled via 2D NiO and N-doped graphene(NG)nanosheets.This procedure can yield nanostructures that satisfy the criteria correlated with improved electrocatalytic performance,such as large surface area,numerous undercoordinated atoms,and high defect densities.Further,porous NG nanosheet architectures,featuring NiO nanosheets densely coordinated with accessible holey Fe_(2)O_(3) moieties,can enhance mesoporosity and balance hydrophilicity.Such improvements can facilitate charge transport and expose formerly inaccessible reaction sites,maximizing active site density utilization.Density functional theory(DFT)calculations reveal favored O_(2) adsorption and dissociation on Fe_(2)O_(3) hybrid structures when supported by 2D NiO and NG nanomaterials,given 2D materials donated charge to Fe_(2)O_(3) active sites.Our systematic studies reveal that synergistic contributions are responsible for enriching the catalytic activity of Fe_(2)O_(3)@NiO/NG in alkaline media-encompassing internal voids and pores,unique hierarchical support structures,and concentrated N-dopant and bimetallic atomic interactions.Ultimately,this work expands the toolbox for designing and synthesizing highly efficient 2D/2D shelled functional nanomaterials with transition metals,endeavoring to benefit energy conversion and related ORR applications.
