期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 24, 期 43, 页码 26556-26563出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cp03740h
关键词
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资金
- Science Challenge Project [TZ2018004]
- National Natural Science Foundation of China [51572016, U1530401, 11704116, 11804090, 51472209, 11774298, U1401241, 21503012]
- project of Hunan Provincial Department of Education [21B0485, 19B206]
- Natural Science Foundation of Hunan Province, China [2019JJ50175, 2019JJ50148]
- Royal Society Newton Advanced Fellowship scheme [NAF\R1\180242]
We systematically studied the influence of p-block atom X (X = C, N, O, S, and Se) on CO2 catalytic properties on a Sn(200) surface and found that the p-block atoms have unique effects on CO2 electrocatalytic activity and product selectivity. In particular, the p-block C atom showed bi-functional activity while the p-block S(Se) atom exhibited strong selectivity towards HCOOH formation. These findings provide valuable insights for the design of highly efficient CO2 electrocatalysts.
Low activity and poor product selectivity of CO2 reduction have seriously hampered its further practical application. Introducing p-block atoms to the catalyst is regarded as a promising strategy due to the versatility of p orbitals and diversity of p-block elements. Here, we systematically studied the influence of p-block atom X (X = C, N, O, S, and Se) on CO2 catalytic properties on a Sn(200) surface by first-principles calculation. Our work shows that all the p-block atoms are relative stable with E-f in the range of -5.11 to -3.59 eV. Further calculation demonstrates that the diversity of the p-block atoms results in unique CO2 electrocatalytic activity and product selectivity. Interestingly, the p-block C atom shows bi-functional activity to form two-electron products HCOOH and CO, with the corresponding energy barriers remarkably low at about 0.19 eV and 0.28 eV. In particular, the p-block S(Se) atom appears to have striking HCOOH selectivity, with the energy barrier to form HCOOH only a quarter of that to form the CO product. This unusual behavior is mainly attributed to the adsorption strength and frontier orbital interaction between the p-block atom and intermediates. These findings can effectively provide a valuable insight into the design of highly efficient CO2 electrocatalyst.
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