The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces c...The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces challenges due to limitations in electrocatalytic activity and durability,especially for nonnoble metal-based catalysts.Here,naturally abundant bismuth-based nanosheets that can effectively drive CO_(2)-to-formate electrocatalytic reduction are prepared using the plasma-activated Bi_(2)Se_(3) followed by a reduction process.Thus-obtained plasma-activated Bi nanosheets(P-BiNS)feature ultrathin structures and high surface areas.Such nanostructures ensure the P-BiNS with outstanding eCO_(2)RR catalytic performance,highlighted by the current density of over 80 mA cm^(-2) and a formate Faradic efficiency of>90%.Furthermore,P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50h of operation.The selectivity for formate production is also studied by density functional theory(DFT)calculations,validating the importance and efficacy of the stabilization of intermediates(^(*)OCHO)on the P-BiNS surfaces.This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.展开更多
The sulfur-containing activated carbons(SACs)were prepared by CO2 activation and sulfur impregnation.The sulfur-containing samples were then oxidized in air.The SACs were characterized by N2 adsorption,elemental analy...The sulfur-containing activated carbons(SACs)were prepared by CO2 activation and sulfur impregnation.The sulfur-containing samples were then oxidized in air.The SACs were characterized by N2 adsorption,elemental analysis,thermogravimetric analysis,X-ray photoelectron spectroscopy,Raman spectroscopy,and X-ray diffraction.The CO2 activation provided precursor carbons with high porosity,which in turn were sulfurized effectively.Oxidation in air at 200℃enlarged pores and redistributed amorphous sulfur in the hierarchical pores.A typical SAC containing 17.89%sulfur exhibited a surface area of 1464 m2/g.This work may open up a valid route to prepare highly microporous SACs with high sulfur loading for applications where the presence of sulfur is beneficial.展开更多
基金partial support from the Jiujiang Research Institute at Xiamen University.
文摘The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces challenges due to limitations in electrocatalytic activity and durability,especially for nonnoble metal-based catalysts.Here,naturally abundant bismuth-based nanosheets that can effectively drive CO_(2)-to-formate electrocatalytic reduction are prepared using the plasma-activated Bi_(2)Se_(3) followed by a reduction process.Thus-obtained plasma-activated Bi nanosheets(P-BiNS)feature ultrathin structures and high surface areas.Such nanostructures ensure the P-BiNS with outstanding eCO_(2)RR catalytic performance,highlighted by the current density of over 80 mA cm^(-2) and a formate Faradic efficiency of>90%.Furthermore,P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50h of operation.The selectivity for formate production is also studied by density functional theory(DFT)calculations,validating the importance and efficacy of the stabilization of intermediates(^(*)OCHO)on the P-BiNS surfaces.This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.
基金Funded by the National Key Technology R&D Program,China(No.2017YFB0307900)。
文摘The sulfur-containing activated carbons(SACs)were prepared by CO2 activation and sulfur impregnation.The sulfur-containing samples were then oxidized in air.The SACs were characterized by N2 adsorption,elemental analysis,thermogravimetric analysis,X-ray photoelectron spectroscopy,Raman spectroscopy,and X-ray diffraction.The CO2 activation provided precursor carbons with high porosity,which in turn were sulfurized effectively.Oxidation in air at 200℃enlarged pores and redistributed amorphous sulfur in the hierarchical pores.A typical SAC containing 17.89%sulfur exhibited a surface area of 1464 m2/g.This work may open up a valid route to prepare highly microporous SACs with high sulfur loading for applications where the presence of sulfur is beneficial.
