Alkaline hydrogen evolution reaction (HER) suffers from a sluggish kinetic,which requires the elaborate catalytic interface and micro-nanoscale architecture engineering of the electrocatalysts to accelerate the water ...Alkaline hydrogen evolution reaction (HER) suffers from a sluggish kinetic,which requires the elaborate catalytic interface and micro-nanoscale architecture engineering of the electrocatalysts to accelerate the water dissociation and hydrogen evolution.Herein,the heterointerface engineering was proposed for promoting the alkaline HER by constructing the highly exposed Ru/RuS_(2) heterostructures homogeneously distributed on hollow N/S-doped carbon microspheres (Ru/RuS_(2)@h-NSC).Benefited from the synergistic effect of heterointerfacial Ru/RuS_(2),the high accessibility of the active sites on both inner and outer surface of mesoporous shells and the efficient mass transport,Ru/RuS_(2)@h-NSC affords a remarkable catalytic performance with an overpotential of 26 mV@10 mA/cm^(2) for alkaline HER,outperforming most of the state-of-the-art catalysts.Further applying Ru/RuS_(2)@h-NSC and its oxidized derivate for the overall alkaline water splitting,the required cell voltage is much lower than that of the commercial Pt/C||RuO_(2)pair to achieve the same current density.Our study may allow us to guide the design of micro-nanoreactors with optimal catalytic interfaces for promising electrocatalytic applications.展开更多
Facile mass transport channel and accessible active sites are crucial for binder-free air electrode catalysts in rechargeable flexible zinc-air battery(ZAB).Herein,a ZnS/NH3 dual-assisted pyrolysis strategy is propose...Facile mass transport channel and accessible active sites are crucial for binder-free air electrode catalysts in rechargeable flexible zinc-air battery(ZAB).Herein,a ZnS/NH3 dual-assisted pyrolysis strategy is proposed to prepare N/S-doped hierarchical porous bamboo carbon cloth(HP-NS-BCC)as binder-free air electrode catalyst for ZAB.BCC fabric with abundant micropores is firstly used as flexible carbon support to facilitate the heteroatom-doping and construct the hierarchical porous structure.ZnS nanospheres and NH3 activization together facilitate the electronic modulation of carbon matrix by N/S-doping and optimize the macro/meso/micropores structure of carbon fibers.Benefiting from the highly-exposed N/S-induced sites with enhanced intrinsic activity,the optimized mass transport of biocarbon fibers,as well as the ultra-large specific surface area of 2436.1 m^(2)·g^(-1),the resultant HP-NS-BCC catalyst exhibits improved kinetics for oxygen reduction/evolution reaction.When applied to rechargeable aqueous ZABs,it achieves a significant peak power density of 249.1 mW·cm^(-2).As binder-free air electrode catalyst,the flexible ZAB also displays stable cycling over 500 cycles with a minimal voltage gap of 0.42 V,showcasing promising applications in flexible electronic devices.展开更多
Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only sh...Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only show good ORR activity in alkaline medium,and become less effective in acidic environment.We believe that an appropriate combination of both ionic and electronic transport path,and well dopant distribution of doped carbon-based materials would help to realize high ORR performance un-der both acidic and alkaline cond让ions.Accordingly,a nitrogen and sulfur co-doped carbon framework with hierarchical through-hole structure is fabricated by morphology-controlled solid-state pyrolysis of poly(aniline-co-2-ami no thiophenol)foam.The uniform high concentrations of nitrogen and sulfur,high intrinsic conductivity,and integrated three dimensional ionic and electronic transfer passageways of the 3D porous structure lead to synergistic effects in catalyzing ORR.As a result,the limiting current density of the carbonized poly(aniline-co-2-aminothiophenol)foam is equivalent to commercial Pt/C in acidic environment,and twice the latter in alkaline medium.展开更多
基金financially supported by the National Key R&D Program of China (No. 2021YFA1500402)the National Natural Science Foundation of China (NSFC, Nos. 21901246, 22105203 and 22175174)the Natural Science Foundation of Fujian Province (Nos. 2020J01116 and 2021J06033)。
文摘Alkaline hydrogen evolution reaction (HER) suffers from a sluggish kinetic,which requires the elaborate catalytic interface and micro-nanoscale architecture engineering of the electrocatalysts to accelerate the water dissociation and hydrogen evolution.Herein,the heterointerface engineering was proposed for promoting the alkaline HER by constructing the highly exposed Ru/RuS_(2) heterostructures homogeneously distributed on hollow N/S-doped carbon microspheres (Ru/RuS_(2)@h-NSC).Benefited from the synergistic effect of heterointerfacial Ru/RuS_(2),the high accessibility of the active sites on both inner and outer surface of mesoporous shells and the efficient mass transport,Ru/RuS_(2)@h-NSC affords a remarkable catalytic performance with an overpotential of 26 mV@10 mA/cm^(2) for alkaline HER,outperforming most of the state-of-the-art catalysts.Further applying Ru/RuS_(2)@h-NSC and its oxidized derivate for the overall alkaline water splitting,the required cell voltage is much lower than that of the commercial Pt/C||RuO_(2)pair to achieve the same current density.Our study may allow us to guide the design of micro-nanoreactors with optimal catalytic interfaces for promising electrocatalytic applications.
基金supported by the National Natural Science Foundation of China(Grant Nos.52102260,22379056,52202243)the project funded by China Postdoctoral Science Foundation(Grant Nos.2022M711545,2022M711371)+1 种基金Research and Practice Innovation Plan of Postgraduate Training Innovation Project in Jiangsu Province(SJCX23_2156)Shanghai Frontiers Research Center of the Hadal Biosphere,SciTech Funding by CSPFTZ Lingang Special Area Marine Biomedical Innovation Platform.
文摘Facile mass transport channel and accessible active sites are crucial for binder-free air electrode catalysts in rechargeable flexible zinc-air battery(ZAB).Herein,a ZnS/NH3 dual-assisted pyrolysis strategy is proposed to prepare N/S-doped hierarchical porous bamboo carbon cloth(HP-NS-BCC)as binder-free air electrode catalyst for ZAB.BCC fabric with abundant micropores is firstly used as flexible carbon support to facilitate the heteroatom-doping and construct the hierarchical porous structure.ZnS nanospheres and NH3 activization together facilitate the electronic modulation of carbon matrix by N/S-doping and optimize the macro/meso/micropores structure of carbon fibers.Benefiting from the highly-exposed N/S-induced sites with enhanced intrinsic activity,the optimized mass transport of biocarbon fibers,as well as the ultra-large specific surface area of 2436.1 m^(2)·g^(-1),the resultant HP-NS-BCC catalyst exhibits improved kinetics for oxygen reduction/evolution reaction.When applied to rechargeable aqueous ZABs,it achieves a significant peak power density of 249.1 mW·cm^(-2).As binder-free air electrode catalyst,the flexible ZAB also displays stable cycling over 500 cycles with a minimal voltage gap of 0.42 V,showcasing promising applications in flexible electronic devices.
基金financial support by the National Natural Science Foundation of China (Grant: 51333008)Young Teacher Training Program of Sun Yat-sen University (Grant: 17lgpy86)
文摘Developing high-performance non-precious metal electrocatalysts for oxygen reduction reaction(ORR)is crucial for the commercialization of fuel cells and metal-air batteries.However,doped carbon-based materials only show good ORR activity in alkaline medium,and become less effective in acidic environment.We believe that an appropriate combination of both ionic and electronic transport path,and well dopant distribution of doped carbon-based materials would help to realize high ORR performance un-der both acidic and alkaline cond让ions.Accordingly,a nitrogen and sulfur co-doped carbon framework with hierarchical through-hole structure is fabricated by morphology-controlled solid-state pyrolysis of poly(aniline-co-2-ami no thiophenol)foam.The uniform high concentrations of nitrogen and sulfur,high intrinsic conductivity,and integrated three dimensional ionic and electronic transfer passageways of the 3D porous structure lead to synergistic effects in catalyzing ORR.As a result,the limiting current density of the carbonized poly(aniline-co-2-aminothiophenol)foam is equivalent to commercial Pt/C in acidic environment,and twice the latter in alkaline medium.
