This study developed a symbiotic dual-confinement strategy integrating interstitial oxygen doping and carbon coating to enhance high-entropy alloys for high-current-density zinc-air batteries.Through the combination o...This study developed a symbiotic dual-confinement strategy integrating interstitial oxygen doping and carbon coating to enhance high-entropy alloys for high-current-density zinc-air batteries.Through the combination of theoretical cluster models with the experimental synthesis of MnFeCoNiCu@C high-entropy alloys,the synergistic suppression of demetalization and kinetic optimization was investigated.The dual-confined high-entropy alloys exhibited no significant attenuation for 1600 h in zinc-air batteries and resisted large current of 100 mA cm^(-2)impacts,with density functional theory calculations confirming lower d-band centers and higher formation energies,correlating with enhanced durability and reaction kinetics.展开更多
Magnesium-lithium hybrid batteries(MLHBs)have gained increasing attention due to their combined advantages of rapid ion insertion/extraction cathode and magnesium metal anode.Herein,Sn S_(2)-SPAN hybrid cathode with s...Magnesium-lithium hybrid batteries(MLHBs)have gained increasing attention due to their combined advantages of rapid ion insertion/extraction cathode and magnesium metal anode.Herein,Sn S_(2)-SPAN hybrid cathode with strong C-Sn bond and rich defects is ingeniously constructed to realize Mg^(2+)/Li^(+)co-intercalation.The physical and chemical double-confinement synergistic engineering of sulfurized polyacrylonitrile can suppress the agglomeration of Sn S_(2)nanoparticles and the volume expansion,simultaneously promote charge transfer and enhance structural stability.The introduced abundant sulfur vacancies provide more active sites for Mg^(2+)/Li^(+)co-intercalation.Meanwhile,the beneficial effects of rich sulfur defects and C-Sn bond on enhanced electrochemical properties are further evidenced by density-functional theory(DFT)calculations.Therefore,compared with pristine SnS_(2),SnS_(2)-SPAN cathode displays high specific capacity(218 m Ah g^(-1)at 0.5A g^(-1)over 700 cycles)and ultra-long cycling life(101 m Ah g^(-1)at 5 A g^(-1)up to 28,000 cycles).And a high energy density of 307 Wh kg^(-1)can be realized by the Sn S_(2)-SPAN//Mg pouch cell.Such elaborate and simple design supplies a reference for the exploitation of advanced cathode materials with excellent electrochemical properties for MLHBs.展开更多
Rationally developing efficient and durable bifunctional catalysts toward oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is critical for rechargeable zinc-air batteries(ZABs).Herein,a bead-like CoSe_(...Rationally developing efficient and durable bifunctional catalysts toward oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is critical for rechargeable zinc-air batteries(ZABs).Herein,a bead-like CoSe_(2)@NC@NCNFs bifunctional catalyst was designed and fabricated by confining cubic CoSe_(2)nanoparticles to three-dimensional(3D)porous MOFs-derived nitrogen-doped carbon(NC)and one-dimensional(1D)N-doped carbon nanofibers(NCNFs)through a facile encapsulate strategy.The 1D/3D continuous network structure contributes to the improvement of specific surface area and electronic conductivity,while the strong synergistic effect between CoSe_(2)sites and Co-Nx-C sites can effectively enhance electron/mass transfer and reduce the diffusion resistance.The as-constructed CoSe_(2)@NC@NCNFs catalyst exhibits high catalytic activity and stability toward ORR/OER with a high half-wave potential of 0.80 V(vs.RHE)in ORR and a low overpotential of 280 mV at 10 mA·cm^(−2)in OER.More encouragingly,the rechargeable ZABs with CoSe_(2)@NC@NCNFs cathode deliver high peak power densities(126.8 mW·cm^(−2)),large specific capacities(763.1 mA·h·g^(−1)),and robust charge-discharge cycling stability over 240 cycles.This study provides a facile strategy for designing efficient bifunctional catalysts for rechargeable energy conversion applications.展开更多
基金financial support provided by the National Natural Science Foundation of Yunnan Province(202301AS070040)Major Science and Technology Projects of Yunnan Province(202302AB080019-3)。
文摘This study developed a symbiotic dual-confinement strategy integrating interstitial oxygen doping and carbon coating to enhance high-entropy alloys for high-current-density zinc-air batteries.Through the combination of theoretical cluster models with the experimental synthesis of MnFeCoNiCu@C high-entropy alloys,the synergistic suppression of demetalization and kinetic optimization was investigated.The dual-confined high-entropy alloys exhibited no significant attenuation for 1600 h in zinc-air batteries and resisted large current of 100 mA cm^(-2)impacts,with density functional theory calculations confirming lower d-band centers and higher formation energies,correlating with enhanced durability and reaction kinetics.
基金financially supported by the National Key R&D Program of China(No.2023YFB3809500)National Natural Science Foundation of China(Grant No.51931006,52272240 and U22A20118)+2 种基金the Fundamental Research Funds for the Central Universities of China(Xiamen University:No.20720220074)Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(HRTP-[2022]-22)the“Double-First Class”Foundation of Materials Intelligent Manufacturing Discipline of Xiamen University。
文摘Magnesium-lithium hybrid batteries(MLHBs)have gained increasing attention due to their combined advantages of rapid ion insertion/extraction cathode and magnesium metal anode.Herein,Sn S_(2)-SPAN hybrid cathode with strong C-Sn bond and rich defects is ingeniously constructed to realize Mg^(2+)/Li^(+)co-intercalation.The physical and chemical double-confinement synergistic engineering of sulfurized polyacrylonitrile can suppress the agglomeration of Sn S_(2)nanoparticles and the volume expansion,simultaneously promote charge transfer and enhance structural stability.The introduced abundant sulfur vacancies provide more active sites for Mg^(2+)/Li^(+)co-intercalation.Meanwhile,the beneficial effects of rich sulfur defects and C-Sn bond on enhanced electrochemical properties are further evidenced by density-functional theory(DFT)calculations.Therefore,compared with pristine SnS_(2),SnS_(2)-SPAN cathode displays high specific capacity(218 m Ah g^(-1)at 0.5A g^(-1)over 700 cycles)and ultra-long cycling life(101 m Ah g^(-1)at 5 A g^(-1)up to 28,000 cycles).And a high energy density of 307 Wh kg^(-1)can be realized by the Sn S_(2)-SPAN//Mg pouch cell.Such elaborate and simple design supplies a reference for the exploitation of advanced cathode materials with excellent electrochemical properties for MLHBs.
基金supported by the National Natural Science Foundation of China(Nos.52174286,22105190)Natural Science Foundation of Hunan Province in China(2023JJ10068)Innovation-Driven Project of Central South University(No.2020CX007).
文摘Rationally developing efficient and durable bifunctional catalysts toward oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)is critical for rechargeable zinc-air batteries(ZABs).Herein,a bead-like CoSe_(2)@NC@NCNFs bifunctional catalyst was designed and fabricated by confining cubic CoSe_(2)nanoparticles to three-dimensional(3D)porous MOFs-derived nitrogen-doped carbon(NC)and one-dimensional(1D)N-doped carbon nanofibers(NCNFs)through a facile encapsulate strategy.The 1D/3D continuous network structure contributes to the improvement of specific surface area and electronic conductivity,while the strong synergistic effect between CoSe_(2)sites and Co-Nx-C sites can effectively enhance electron/mass transfer and reduce the diffusion resistance.The as-constructed CoSe_(2)@NC@NCNFs catalyst exhibits high catalytic activity and stability toward ORR/OER with a high half-wave potential of 0.80 V(vs.RHE)in ORR and a low overpotential of 280 mV at 10 mA·cm^(−2)in OER.More encouragingly,the rechargeable ZABs with CoSe_(2)@NC@NCNFs cathode deliver high peak power densities(126.8 mW·cm^(−2)),large specific capacities(763.1 mA·h·g^(−1)),and robust charge-discharge cycling stability over 240 cycles.This study provides a facile strategy for designing efficient bifunctional catalysts for rechargeable energy conversion applications.
