HNO 3 -pretreated CNTs were employed as supports, and a special ultrasound-assisted impregnation method was designed to prepare supported Cu-Co catalysts for higher-alcohol synthesis from syngas. The catalysts used in...HNO 3 -pretreated CNTs were employed as supports, and a special ultrasound-assisted impregnation method was designed to prepare supported Cu-Co catalysts for higher-alcohol synthesis from syngas. The catalysts used in this work were characterized by N 2 adsorption-desorption, TEM, XRD, H 2 -TPR, CO-TPD techniques. It was found that the pre-treatment procedure of CNTs remarkably promoted the catalytic properties of the Cu-Co/CNTs catalysts. For the Cu-Co catalyst supported on CNTs pre-treated by 68 wt% HNO 3 , some active components were introduced into the CNTs channels, their dispersions and the amount of strongly adsorbed CO-species were improved. The CO conversion and alcohol yield on the HNO 3 -pretreated Cu-Co/CNTs catalyst were increased by ～21% and ～69%, respectively, compared with those on the normal Cu-Co/CNTs catalyst.展开更多
Electrocatalytic conversion of renewable biomass is emerging as a promising route for sustainable chemical production;hence it urgently calls for developing efficient electrocatalysts with low potentials and high curr...Electrocatalytic conversion of renewable biomass is emerging as a promising route for sustainable chemical production;hence it urgently calls for developing efficient electrocatalysts with low potentials and high current densities.Herein,a Pr-doped Co(OH)_(2)hexagonal sheet(Pr/Co=1/9,in mole)is synthesized by electrodeposition as highly performant catalyst for 5-hydroxymethylfurfural(HMF)oxidation reaction(HMFOR)to produce 2,5-furandicarboxylic acid(FDCA).This novel and low-cost catalyst possesses a rather low onset potential of 1.05 V(vs.RHE)and requires only 1.10 V(vs.RHE)to reach a current density of 10 mA cm^(-2)for HMFOR,significantly outperforming Co(OH)_(2)benchmark(i.e.,210 mV higher to reach10 m A cm^(-2)).The origin of Pr promotion effect as well as the evolution of CoOOH catalytic sites and HMFOR process has been deeply elucidated by physical characterizations,kinetic experiments,in situ electrochemical techniques,and theoretical calculations.The unique Pr-ameliorated CoOOH active centers enable 100%conversion of HMF,99.6%selectivity of FDCA,and 99.7%Faraday efficiency,with a superior cycling durability toward HMFOR.This can be one of the most outstanding results for Co-based HMFOR catalysts to date in the literature.Thereby this work can help open up new horizons for constructing novel and efficient Co-based electrocatalysts by the utilization of lanthanide elements.展开更多
基金supported by the Foundation of Shaanxi Educational Committee (2010JK608)the Research Foundation of XATU (204-000092)supported by the National Natural Science Foundation of China (205903603)
文摘HNO 3 -pretreated CNTs were employed as supports, and a special ultrasound-assisted impregnation method was designed to prepare supported Cu-Co catalysts for higher-alcohol synthesis from syngas. The catalysts used in this work were characterized by N 2 adsorption-desorption, TEM, XRD, H 2 -TPR, CO-TPD techniques. It was found that the pre-treatment procedure of CNTs remarkably promoted the catalytic properties of the Cu-Co/CNTs catalysts. For the Cu-Co catalyst supported on CNTs pre-treated by 68 wt% HNO 3 , some active components were introduced into the CNTs channels, their dispersions and the amount of strongly adsorbed CO-species were improved. The CO conversion and alcohol yield on the HNO 3 -pretreated Cu-Co/CNTs catalyst were increased by ～21% and ～69%, respectively, compared with those on the normal Cu-Co/CNTs catalyst.
基金National Natural Science Foundation of China(No.22272149,22062025)Yunnan University’s Research Innovation Fund for Graduate Students(No.KC-23234085)+1 种基金Workstation of Academician Chen Jing of Yunnan Province(No.202105AF150012)Free Exploration Fund for Academician(No.202405AA350001)。
文摘Electrocatalytic conversion of renewable biomass is emerging as a promising route for sustainable chemical production;hence it urgently calls for developing efficient electrocatalysts with low potentials and high current densities.Herein,a Pr-doped Co(OH)_(2)hexagonal sheet(Pr/Co=1/9,in mole)is synthesized by electrodeposition as highly performant catalyst for 5-hydroxymethylfurfural(HMF)oxidation reaction(HMFOR)to produce 2,5-furandicarboxylic acid(FDCA).This novel and low-cost catalyst possesses a rather low onset potential of 1.05 V(vs.RHE)and requires only 1.10 V(vs.RHE)to reach a current density of 10 mA cm^(-2)for HMFOR,significantly outperforming Co(OH)_(2)benchmark(i.e.,210 mV higher to reach10 m A cm^(-2)).The origin of Pr promotion effect as well as the evolution of CoOOH catalytic sites and HMFOR process has been deeply elucidated by physical characterizations,kinetic experiments,in situ electrochemical techniques,and theoretical calculations.The unique Pr-ameliorated CoOOH active centers enable 100%conversion of HMF,99.6%selectivity of FDCA,and 99.7%Faraday efficiency,with a superior cycling durability toward HMFOR.This can be one of the most outstanding results for Co-based HMFOR catalysts to date in the literature.Thereby this work can help open up new horizons for constructing novel and efficient Co-based electrocatalysts by the utilization of lanthanide elements.
