Ke Jingwen, Zhao Jiankang, Chi Mingfang, Wang Menglin, Kong Xiangdong, Chang Qixuan, Zhou Weiran, Long Chengxuan, Zeng Jie, Geng Zhigang
Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Nat Commun. 2022 Feb 17;13(1):932. doi: 10.1038/s41467-022-28516-0.
The electrooxidation of propylene into propylene oxide under ambient conditions represents an attractive approach toward propylene oxide. However, this process suffers from a low yield rate over reported electrocatalysts. In this work, we develop an efficient electrocatalyst of AgPO for the electrooxidation of propylene into propylene oxide. The AgPO cubes with (100) facets exhibit the highest yield rate of 5.3 g m h at 2.4 V versus reversible hydrogen electrode, which is 1.6 and 2.5 times higher than those over AgPO rhombic dodecahedra with (110) facets and tetrahedra with (111) facets, respectively. The theoretical calculations reveal that the largest polarization of propylene on AgPO (100) facets is beneficial to break the symmetric π bonding and facilitate the formation of C-O bond. Meanwhile, AgPO(100) facets exhibit the lowest adsorption energies of CH and OH, inducing the lowest energy barrier of the rate-determining step and thus accounting for the highest catalytic performance.
在环境条件下将丙烯电氧化为环氧丙烷是一种制备环氧丙烷的有吸引力的方法。然而，在已报道的电催化剂上，该过程的产率较低。在这项工作中，我们开发了一种用于将丙烯电氧化为环氧丙烷的高效电催化剂AgPO。具有（100）晶面的AgPO立方体在相对于可逆氢电极2.4 V的电压下表现出最高产率，为5.3 g m⁻² h⁻¹，分别比具有（110）晶面的AgPO菱形十二面体和具有（111）晶面的四面体高出1.6倍和2.5倍。理论计算表明，丙烯在AgPO（100）晶面上的最大极化有利于打破对称π键并促进C-O键的形成。同时，AgPO（100）晶面表现出最低的CH和OH吸附能，导致速率决定步骤的能垒最低，从而具有最高的催化性能。
