CO_(2)electrochemical reduction(CO_(2)ER)to high-value fuels and chemicals is a promising strategy for using CO_(2)as a carbon source.However,the large-scale application of CO_(2)ER is limited by the lack of efficient...CO_(2)electrochemical reduction(CO_(2)ER)to high-value fuels and chemicals is a promising strategy for using CO_(2)as a carbon source.However,the large-scale application of CO_(2)ER is limited by the lack of efficient and selective electrocatalysts.By means of density functional theory(DFT)calculations,the potential of transitional metal-based covalent organic frameworks(TM-COFs,TM=Fe,Co,Ni,Cu,Zn,Ru,Rh,Pd,and Ag)as CO_(2)reduction electrocatalysts was systematically studied.The results show that the single TM atom can be firmly anchored on COFs for forming stable single-atom catalysts.The TM atom in phthalocyanine has excellent catalytic activity towards CO_(2)ER,while the pyridine N in pyrazine is the active site of the hydrogen evolution reaction(HER).Among studied candidates,Co-COF and Rh-COF are predicted to have limiting potential of-0.66/-0.11 and-0.49/-0.49 V for CO_(2)ER/HER,respectively.The present study may provide a new strategy for designing novel bifunctional catalysts.展开更多
基金the financial support by the Natural Science Foundation of Science and Technology Department of Jilin Province(20210101131JC)the Education Department of Jilin Province(JJKH20230217KJ).
文摘CO_(2)electrochemical reduction(CO_(2)ER)to high-value fuels and chemicals is a promising strategy for using CO_(2)as a carbon source.However,the large-scale application of CO_(2)ER is limited by the lack of efficient and selective electrocatalysts.By means of density functional theory(DFT)calculations,the potential of transitional metal-based covalent organic frameworks(TM-COFs,TM=Fe,Co,Ni,Cu,Zn,Ru,Rh,Pd,and Ag)as CO_(2)reduction electrocatalysts was systematically studied.The results show that the single TM atom can be firmly anchored on COFs for forming stable single-atom catalysts.The TM atom in phthalocyanine has excellent catalytic activity towards CO_(2)ER,while the pyridine N in pyrazine is the active site of the hydrogen evolution reaction(HER).Among studied candidates,Co-COF and Rh-COF are predicted to have limiting potential of-0.66/-0.11 and-0.49/-0.49 V for CO_(2)ER/HER,respectively.The present study may provide a new strategy for designing novel bifunctional catalysts.
