Electrochemical coupling hydrogen evolution with biomass reforming reaction(named electrochemical hydrogen and chemical cogeneration(EHCC)),which realizes green hydrogen production and chemical upgrading simultaneousl...Electrochemical coupling hydrogen evolution with biomass reforming reaction(named electrochemical hydrogen and chemical cogeneration(EHCC)),which realizes green hydrogen production and chemical upgrading simultaneously,is a promising method to build a carbon-neutral society.Herein,we analyze the EHCC process by considering the market assessment.The ethanol to acetic acid and hydrogen approach is the most feasible for large-scale hydrogen production.We develop AuCu nanocatalysts,which can selectively oxidize ethanol to acetic acid(>97%)with high long-term activity.The isotopic and in-situ infrared experiments reveal that the promoted water dissociation step by alloying contributes to the enhanced activity of the partial oxidation reaction path.A flow-cell electrolyzer equipped with the AuCu anodic catalyst achieves the steady production of hydrogen and acetic acid simultaneously in both high selectivity(>90%),demonstrating the potential scalable application for green hydrogen production with low energy consumption and high profitability.展开更多
Electrochemical upgrading of biomass ethanol to value-added chemicals is promising for sustainable society.Here,we synthesize defective Ni_(3)S_(2) nanowires(NWs),which show high activity towards electrochemical oxida...Electrochemical upgrading of biomass ethanol to value-added chemicals is promising for sustainable society.Here,we synthesize defective Ni_(3)S_(2) nanowires(NWs),which show high activity towards electrochemical oxidation of ethanol to acetate.The Ni_(3)S_(2) NWs are formed by the oriented attachment mechanism,and rich defects are introduced during the growth.A low onset potential of 1.31 V and high mass activity of 8,716 mA·mgNi^(-1) at 1.5 V are achieved using the synthesized Ni_(3)S_(2) NWs toward the ethanol electro-oxidation,which are better than the Ni(OH)2 NWs and the Ni_(3)S_(2) nanoparticles(NPs).And the selectivity for the acetate generation is ca.99%.The high activity of Ni_(3)S_(2) NWs is attributed to the easier oxidation of Ni(II)to the catalytically active Ni(III)species with the promotion from S component and rich defects.These results demonstrate that the defective NWs can be synthesized by the oriented attachment method and the defective Ni_(3)S_(2) NWs structure as the efficient nonnoble metal electrocatalysts for oxidative upgrading of ethanol.展开更多
The development of efficient and cost-effective oxygen evolution reaction(OER)electrocatalysts is crucial for clean energy conversion and storage devices,such as water-splitting,CO_(2) reduction,and metalair batteries...The development of efficient and cost-effective oxygen evolution reaction(OER)electrocatalysts is crucial for clean energy conversion and storage devices,such as water-splitting,CO_(2) reduction,and metalair batteries.Herein,we report an efficient 2-dimensional OER catalyst of ultrathin nickel-iron sulfide nanosheets(Ni Fe S-NS).Dodecanethiol is employed in the synthesis,which prohibits the growth along the Z-axis,thus a nanosheet is obtained.The Ni Fe S-NS shows high OER catalytic activity,which only requires a small overpotential of 273 mV to achieve the OER current density of 10 mA/cm^(2) in alkaline electrolyte,and almost no decay after 150 h of chronopotentiometry test.The high performance is attributed to the 2-dimensional structure,the synergistic effect from the Ni and Fe components which promotes the formation of the high valence Ni species,and the tuning effect from the in-situ generated sulfate doping.This work demonstrates the advantages of the 2-dimensional sulfides in electrocatalysis.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21971008 and 22279004)Beijing Natural Science Foundation(No.Z210016)Fundamental Research Funds for the Central Universities(No.buctrc201916).
文摘Electrochemical coupling hydrogen evolution with biomass reforming reaction(named electrochemical hydrogen and chemical cogeneration(EHCC)),which realizes green hydrogen production and chemical upgrading simultaneously,is a promising method to build a carbon-neutral society.Herein,we analyze the EHCC process by considering the market assessment.The ethanol to acetic acid and hydrogen approach is the most feasible for large-scale hydrogen production.We develop AuCu nanocatalysts,which can selectively oxidize ethanol to acetic acid(>97%)with high long-term activity.The isotopic and in-situ infrared experiments reveal that the promoted water dissociation step by alloying contributes to the enhanced activity of the partial oxidation reaction path.A flow-cell electrolyzer equipped with the AuCu anodic catalyst achieves the steady production of hydrogen and acetic acid simultaneously in both high selectivity(>90%),demonstrating the potential scalable application for green hydrogen production with low energy consumption and high profitability.
基金financially supported by the National Key Research and Development Program of China (2017YFA0206500)the National Natural Science Foundation of China (21671014)the Fundamental Research Funds for the Central Universities (buctrc201823)
基金This work was supported by the National Natural Science Foundation of China(No.21971008)the Fundamental Research Funds for the Central Universities(buctrc201916,buctrc201823).
文摘Electrochemical upgrading of biomass ethanol to value-added chemicals is promising for sustainable society.Here,we synthesize defective Ni_(3)S_(2) nanowires(NWs),which show high activity towards electrochemical oxidation of ethanol to acetate.The Ni_(3)S_(2) NWs are formed by the oriented attachment mechanism,and rich defects are introduced during the growth.A low onset potential of 1.31 V and high mass activity of 8,716 mA·mgNi^(-1) at 1.5 V are achieved using the synthesized Ni_(3)S_(2) NWs toward the ethanol electro-oxidation,which are better than the Ni(OH)2 NWs and the Ni_(3)S_(2) nanoparticles(NPs).And the selectivity for the acetate generation is ca.99%.The high activity of Ni_(3)S_(2) NWs is attributed to the easier oxidation of Ni(II)to the catalytically active Ni(III)species with the promotion from S component and rich defects.These results demonstrate that the defective NWs can be synthesized by the oriented attachment method and the defective Ni_(3)S_(2) NWs structure as the efficient nonnoble metal electrocatalysts for oxidative upgrading of ethanol.
基金supported by the National Key Research and Development Program of China(No.2019YFA0210300)National Natural Science Foundation of China(No.21971008)Fundamental Research Funds for the Central Universities(Nos.buctrc201916,buctrc201823)。
文摘The development of efficient and cost-effective oxygen evolution reaction(OER)electrocatalysts is crucial for clean energy conversion and storage devices,such as water-splitting,CO_(2) reduction,and metalair batteries.Herein,we report an efficient 2-dimensional OER catalyst of ultrathin nickel-iron sulfide nanosheets(Ni Fe S-NS).Dodecanethiol is employed in the synthesis,which prohibits the growth along the Z-axis,thus a nanosheet is obtained.The Ni Fe S-NS shows high OER catalytic activity,which only requires a small overpotential of 273 mV to achieve the OER current density of 10 mA/cm^(2) in alkaline electrolyte,and almost no decay after 150 h of chronopotentiometry test.The high performance is attributed to the 2-dimensional structure,the synergistic effect from the Ni and Fe components which promotes the formation of the high valence Ni species,and the tuning effect from the in-situ generated sulfate doping.This work demonstrates the advantages of the 2-dimensional sulfides in electrocatalysis.
