For electrochemical carbon dioxide reduction(CO_(2)RR),CO_(2)-to-CO conversion is considered an ideal route towards carbon neutrality for practical applications.Gold(Au)is known as a promising catalyst with high selec...For electrochemical carbon dioxide reduction(CO_(2)RR),CO_(2)-to-CO conversion is considered an ideal route towards carbon neutrality for practical applications.Gold(Au)is known as a promising catalyst with high selectivity for CO;however,it suffers from high cost and low mass-specific activity.In this study,we design and prepare a catalyst featuring uniform S-doped Au nanoparticles on N-doped carbon support(denoted as S-Au/NC)by an in situ synthesis strategy using biomolecules.The S-Au/NC displays high activity and selectivity for CO in CO_(2)RR with a Au loading as low as 0.4 wt.%.The Faradaic efficiency of CO(FECO)for S-Au/NC is above 95%at−0.75 V(vs.RHE);by contrast,the FECO of Au/NC(without S)is only 58%.The Tafel slope is 77.4 mV·dec−1,revealing a favorable kinetics process.Furthermore,S-Au/NC exhibits an excellent long-term stability for CO_(2)RR.Density functional theory(DFT)calculations reveal that the S dopant can boost the activity by reducing the free energy change of the potential-limiting step(formation of the*COOH intermediate).This work not only demonstrates a model catalyst featuring significantly reduced use of noble metals,but also establishes an in situ synthesis strategy for preparing high-performance catalysts.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52072260,21931007,21790052,and U21A20317)the Science and Technology Support Program for Youth Innovation in Universities of Shangdong Province(No.2020KJA012)+2 种基金the Tianjin Natural Science Foundation(Nos.21JCZXJC00130 and B2021201074)the Haihe Laboratory of Sustainable Chemical Transformations,National Key R&D Program of China(No.2017YFA0700104)the University Synergy Innovation Program of Anhui Province(No.GXXT-2020-001).
文摘For electrochemical carbon dioxide reduction(CO_(2)RR),CO_(2)-to-CO conversion is considered an ideal route towards carbon neutrality for practical applications.Gold(Au)is known as a promising catalyst with high selectivity for CO;however,it suffers from high cost and low mass-specific activity.In this study,we design and prepare a catalyst featuring uniform S-doped Au nanoparticles on N-doped carbon support(denoted as S-Au/NC)by an in situ synthesis strategy using biomolecules.The S-Au/NC displays high activity and selectivity for CO in CO_(2)RR with a Au loading as low as 0.4 wt.%.The Faradaic efficiency of CO(FECO)for S-Au/NC is above 95%at−0.75 V(vs.RHE);by contrast,the FECO of Au/NC(without S)is only 58%.The Tafel slope is 77.4 mV·dec−1,revealing a favorable kinetics process.Furthermore,S-Au/NC exhibits an excellent long-term stability for CO_(2)RR.Density functional theory(DFT)calculations reveal that the S dopant can boost the activity by reducing the free energy change of the potential-limiting step(formation of the*COOH intermediate).This work not only demonstrates a model catalyst featuring significantly reduced use of noble metals,but also establishes an in situ synthesis strategy for preparing high-performance catalysts.
