Carbon-based air cathodes offer low cost,high electrical conductivity,and structural tunability.However,they suffer from limited catalytic activity and inefficient gas transport,and they typically rely on noble metal ...Carbon-based air cathodes offer low cost,high electrical conductivity,and structural tunability.However,they suffer from limited catalytic activity and inefficient gas transport,and they typically rely on noble metal additives or complex multilayer configurations.To tackle these issues,this study devised a self-activated integrated carbon-based air cathode.By integrating in situ catalytic site construction with structural optimization,the strategy not only induces the formation of oxygen functional groups(─C─OH,─C═O,─COOH),hierarchical pores,and uniformly distributed active sites,but also establishes a favorable electronic and mass-transport environment.Furthermore,the roll-pressing-based integrated design streamlines electrode construction,reinforces interfacial bonding,and significantly enhances mechanical stability.Density functional theory(DFT)calculations show that oxygen functional groups initiate hydrogen bonding interaction and promote charge enrichment,which improves the activity of the cathode and facilitates intermediate adsorption/desorption in oxygen reduction and evolution reactions processes.As a result,the integrated air cathode-based rechargeable zinc-air batteries(RZABs)achieve a high specific capacity of 811 mAh g^(-1).It also performs well in quasi-solid-state RZABs and silicon-air batteries systems across a wide temperature range,demonstrating strong adaptability and application potential.This study provides a scalable and cost-effective design strategy for high-performance carbon-based air cathodes,offering new insights into advancing durable and practical metal-air energy systems.展开更多
Tin(Sn)is considered an effective anode material for stripping and plating due to its promising capacity,isotropic deposition,and relatively negative redox potential of-0.91 V vs.standard hydrogen electrode(SHE).Howev...Tin(Sn)is considered an effective anode material for stripping and plating due to its promising capacity,isotropic deposition,and relatively negative redox potential of-0.91 V vs.standard hydrogen electrode(SHE).However,the challenges of hydrogen evolution corrosion and“dead Sn”formation at the Snalkaline electrolyte interface restrict its reversibility,which poses challenges for flexible devices and in a broad temperature range.In this study,we successfully designed a corrosion-resistant Sn anode(CuPVDF@Sn)featuring a multilevel microchannel structure.The Sn-affinitive Cu mesh with good electronic conductivity lowers the nucleation energy barrier and enhances deposition uniformity,while PVDF improves hydrogen evolution potential.Additionally,the soft Cu mesh and PVDF provide flexibility in design.As a result,the flexible Cu-PVDF@Sn anode achieves a coulombic efficiency(CE)of 92.61% and stable cycling for over 800 h.The flexible Sn-air battery based on this anode exhibits an energy density of 504 Wh kg^(-1),a peak power density of 80 mW cm^(-2),and a cycling stability of 120 h at 5 mA cm^(-2).It also operates effectively within a wide temperature range of -15-60℃,providing strong support for excellent environmental adaptability.The proposed concept in this work might provide a promising alternative for developing stable Sn anodes in flexible Sn-air batteries.展开更多
基金funded by the National Nature Science Foundation of China(62264006,62574102)“Thousand Talents Program”of Yunnan Province for Young Talents,Innovative Research Teams(in Science and Technology)in the University of Yunnan Province(IRTSTYN),XingDian Talent Support Program for Young Talents,and Frontier Research Team of Kunming University 2023,The Basic Research Project of Yunnan Province(Nos.202201AU070022)+2 种基金Kunming University Talent Introduction Fund(Nos.YJL20024)Yunnan Province Education Department Scientific Research Fund Project(Nos.2024Y759)Undergraduate Innovation and Entrepreneurship Training Program Project of Yunnan Provincial(202411393005)。
文摘Carbon-based air cathodes offer low cost,high electrical conductivity,and structural tunability.However,they suffer from limited catalytic activity and inefficient gas transport,and they typically rely on noble metal additives or complex multilayer configurations.To tackle these issues,this study devised a self-activated integrated carbon-based air cathode.By integrating in situ catalytic site construction with structural optimization,the strategy not only induces the formation of oxygen functional groups(─C─OH,─C═O,─COOH),hierarchical pores,and uniformly distributed active sites,but also establishes a favorable electronic and mass-transport environment.Furthermore,the roll-pressing-based integrated design streamlines electrode construction,reinforces interfacial bonding,and significantly enhances mechanical stability.Density functional theory(DFT)calculations show that oxygen functional groups initiate hydrogen bonding interaction and promote charge enrichment,which improves the activity of the cathode and facilitates intermediate adsorption/desorption in oxygen reduction and evolution reactions processes.As a result,the integrated air cathode-based rechargeable zinc-air batteries(RZABs)achieve a high specific capacity of 811 mAh g^(-1).It also performs well in quasi-solid-state RZABs and silicon-air batteries systems across a wide temperature range,demonstrating strong adaptability and application potential.This study provides a scalable and cost-effective design strategy for high-performance carbon-based air cathodes,offering new insights into advancing durable and practical metal-air energy systems.
基金funded by the National Nature Science Foundation of China(62264006)the Special Basic Cooperative Research Programs of Yunnan Provincial Undergraduate Universities’Association(202101BA070001-034)+1 种基金the“Thousand Talents Program”of Yunnan Province for Young Talents,XingDian Talent Support Program for Young TalentsFrontier Research Team of Kunming University 2023。
文摘Tin(Sn)is considered an effective anode material for stripping and plating due to its promising capacity,isotropic deposition,and relatively negative redox potential of-0.91 V vs.standard hydrogen electrode(SHE).However,the challenges of hydrogen evolution corrosion and“dead Sn”formation at the Snalkaline electrolyte interface restrict its reversibility,which poses challenges for flexible devices and in a broad temperature range.In this study,we successfully designed a corrosion-resistant Sn anode(CuPVDF@Sn)featuring a multilevel microchannel structure.The Sn-affinitive Cu mesh with good electronic conductivity lowers the nucleation energy barrier and enhances deposition uniformity,while PVDF improves hydrogen evolution potential.Additionally,the soft Cu mesh and PVDF provide flexibility in design.As a result,the flexible Cu-PVDF@Sn anode achieves a coulombic efficiency(CE)of 92.61% and stable cycling for over 800 h.The flexible Sn-air battery based on this anode exhibits an energy density of 504 Wh kg^(-1),a peak power density of 80 mW cm^(-2),and a cycling stability of 120 h at 5 mA cm^(-2).It also operates effectively within a wide temperature range of -15-60℃,providing strong support for excellent environmental adaptability.The proposed concept in this work might provide a promising alternative for developing stable Sn anodes in flexible Sn-air batteries.
