标题：Understanding the enhanced catalytic activity of bimetallic AuCu/TiO(2)in CO(2)adsorption and activation: a density functional theory study
作者：Liu, Li; Lv, Pingli
作者机构：[Liu, Li; Lv, Pingli] Qilu Univ Technol, Shandong Acad Sci, Sch Light Ind & Engn, Jinan 250353, Peoples R China.; [Liu, Li] Qilu Univ Technol, Key L 更多
通讯作者：Liu, Li;Liu, Li
通讯作者地址：Liu, L (corresponding author), Qilu Univ Technol, Shandong Acad Sci, Sch Light Ind & Engn, Jinan 250353, Peoples R China.; Liu, L (corresponding autho 更多
来源：NEW JOURNAL OF CHEMISTRY
摘要：Photoreduction of CO(2)to hydrocarbons has lately attracted increased attention. Understanding the reaction mechanism of photocatalytic reduction of CO(2)is crucial for the development of CO(2)photocatalysts. CO(2)adsorption and activation are the first steps of CO(2)photoreduction. In this work, the adsorption and activation of CO(2)on TiO2-supported Au and Au-Cu clusters were studied using density functional theory (DFT) calculations to identify the key factors for improving its adsorption and activation. The presence of Cu atoms was found to have great significance in the adsorption and activation of CO2, and the Cu7 atom on the Au7Cu3/TiO2(101) surface exhibited the strongest CO(2)adsorption ability. By analyzing the surface electronic structure, we found that the up-shift of the d-band center toward the Fermi level in the presence of Cu atoms increased the binding strength of CO2. Additionally, the Cu atoms were positively charged on the Au7Cu3/TiO2(101) surface and promoted the adsorption of CO(2)by increasing the electrostatic attraction between the O atom of CO(2)and the Cu atom. Therefore, compared to the Au-10/TiO2(101) surface, the activity of the Au7Cu3/TiO2(101) surface can be definitely improved. Our results can provide useful insights into the design and development of more efficient bimetallic cluster supported TiO(2)photocatalysts, which are used as catalysts for the synthesis of hydrocarbon fuels by CO(2)hydrogenation.