| Autor: |
Tang BW; School of Physics and Electronic Science, Hunan University of Science and Technology, Xiangtan 411201, China. 1081003@hnust.edu.cn.; Key Laboratory of Intelligent Sensors and Advanced Sensing Materials of Hunan Province, Hunan University of Science and Technology, Xiangtan 411201, China., Liu Y; School of Physics and Electronic Science, Hunan University of Science and Technology, Xiangtan 411201, China. 1081003@hnust.edu.cn., Deng DW; School of Physics and Electronic Science, Hunan University of Science and Technology, Xiangtan 411201, China. 1081003@hnust.edu.cn., Xu Y; School of Physics and Electronic Science, Hunan University of Science and Technology, Xiangtan 411201, China. 1081003@hnust.edu.cn., Wen B; School of Physics and Electronics, Henan University, Kaifeng 475001, P. R. China., Tang ZK; College of Physics and Electronics Engineering, Hengyang Normal University, Hengyang 421008, China., Wei XL; Department of Physics and Laboratory for Quantum Engineering and Micro-Nano Energy Technology, Xiangtan University, Xiangtan 411105, Hunan, China., Ge QX; School of Physics and Electronic Science, Hunan University of Science and Technology, Xiangtan 411201, China. 1081003@hnust.edu.cn., Yin WJ; School of Physics and Electronic Science, Hunan University of Science and Technology, Xiangtan 411201, China. 1081003@hnust.edu.cn.; Key Laboratory of Intelligent Sensors and Advanced Sensing Materials of Hunan Province, Hunan University of Science and Technology, Xiangtan 411201, China. |
| Abstrakt: |
Low activity and poor product selectivity of CO 2 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 CO 2 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 CO 2 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 CO 2 electrocatalyst. |
