摘要
The conversion of CO_(2)into fuels and valuable chemicals presents a viable path toward carbon neutrality.The aim of this study is to investigate the potential of metal-doped graphene catalysts in the reduction of CO_(2)to C_(1)products.20 typical M-graphene(M=metal)catalysts were established based on DFT calculations.Six candidate catalysts,i.e.,V-,Cr-,Mn-,Ni-,Mo-,and Ta-graphene catalysts,were selected by combining the hydrogen dissociation ability and the energy band gap of the catalysts.Subsequently,the adsorption characteristics and hydrogenation reactions of CO_(2)over the six candidates were explored.CO_(2)tends to adsorb at the M site through vertical adsorption and car-bon–oxygen co-adsorption.V-and Cr-graphene catalysts promote the production of intermediate COOH,whereas Mn-,Ni-,Mo-,and Ta-doped surfaces are more favorable for HCOO formation.Concerning the hydrogenation to CO and HCOOH,V-,Cr-,Ni-and Mo-graphene catalysts preferentially yield CO from COOH,whereas Ta-doped graphene favors the formation of HCOOH.In total,the competitive hydrogenation of CO_(2)reveals the selectivity of the C_(1)products.Cr-and Ni-graphene favor the production of HCOOH and CH_(3)OH,whereas V-,Mn-,Mo-,and Ta-graphene primarily yield CH_(3)OH.
基金
the National Natural Science Foundation of China(52276189,52376182,52106241)
Natural Science Foundation of Jiangsu Province(BK20221248)
Fundamental Research Funds for the Central Universities(2023JC009)
Project of National Center for International Research on Intelligent Nano-Materials and Detection Technology in Environmental Protection,Soochow University(SDGH2201)for financial support.
