文献类型：期刊文献

英文题名：Structural Shrinking and Rotation Decrease Quasi Surface Tension for Polar CeO2(100)

作者：Zhou, Hui[1,2,3];Wu, Xin-Ping[1,2,3];Gong, Xue-Qing[1,2,3]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem & Mol Engn, Ctr Computat Chem,Joint Int Res Lab Precis Chem &, Feringa Nobel Prize Scientist Joint Res Ctr,Front, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Res Inst Ind Catalysis, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2022

卷号：5

期号：8

外文期刊名：ADVANCED THEORY AND SIMULATIONS

收录：;EI(收录号：20222512250054);WOS:【SCI-EXPANDED(收录号:WOS:000813643900001)】；

基金：This work was supported by National Key R&D Program of China (2018YFA0208602), National Natural Science Foundation of China (21825301, 92045303), the Fundamental Research Funds for the Central Universities (222201717003), Shanghai Municipal Science and Technology Major Project (2018SHZDZX03) and the Programme of Introducing Talents of Discipline to Universities (B16017).

语种：英文

外文关键词：cerium dioxide; density functional theory; polar surfaces; single atom catalysts; surface reconstruction

摘要：Surfaces determine many important physicochemical properties of the solid materials, and the polar surfaces are particularly appealing for their unusual characteristics as they are intrinsically unstable and always reconstruct to compensate for the surface polarity. In this work, by performing density functional theory calculations corrected by on-site Coulomb interactions (DFT+U), it is determined that for polar CeO2 (100), besides the classical O-t, Ce-t, and CeO4-t types of reconstruction, a series of novel "pocket-like" structures can give significantly better stabilities. It is proposed that the shrinking effect caused by the pocket formation can effectively reduce the surface tension, and specifically, promote the rotation of the CeO4 units at CeO4-t-p surface to further stabilize the edge Ce cations of the units. Such CeO4-t-p reconstructed CeO2 (100) can also act as a promising support for the single metal atoms since the induced shrinking and rotation effects can further promote their adsorption and dispersion. This work provides new models to help understand surface reconstruction and adsorption.