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Reaction pathways and the role of the carbonates during CO2 hydrogenation over hexagonal In2O3 catalysts
Applied Surface Science ( IF 6.7 ) Pub Date : 2021-03-01 , DOI: 10.1016/j.apsusc.2020.148591
Bin Qin , Zhimin Zhou , Shenggang Li

Abstract Complete reaction pathways for CO2 hydrogenation to CH3OH and CO on the h-In2O3(0 1 2) and h-In2O3(1 0 4) flat and step surfaces are investigated by density functional theory (DFT) calculations. By analyzing the complete reaction pathways, bi-HCOO* hydrogenation to H2COO* is found to be the rate-determining step (RDS) for CH3OH formation on the h-In2O3(0 1 2) flat surface and h-In2O3(1 0 4) flat and step surfaces, OH* protonation to H2O* is determined as the RDS for CH3OH formation on the h-In2O3(0 1 2) step surface and that for CO formation on the h-In2O3(0 1 2) flat and step surfaces, and bent CO2 configuration (bt-CO2*) protonation to COOH* is predicted to be the RDS for CO formation on the h-In2O3(1 0 4) flat and step surfaces. On the h-In2O3(0 1 2) step surface and the h-In2O3(1 0 4) flat and step surfaces, the carbonate(carb-CO2*) as one of CO2 adsorption configurations can be seen as a spectator species at the Ov sites during the reaction, whereas on the h-In2O3(0 1 2) flat surface, protonation of the carb-CO2* contributes more to CO formation than protonation of the bt-CO2*. Meanwhile, the Ov sites on the h-In2O3(0 1 2) and h-In2O3(1 0 4) step surfaces show lower catalytic activities than corresponding flat surfaces, and thus they are predicted to play little role in determining the catalytic activity of the hexagonal In2O3 catalysts.

中文翻译:

反应途径和碳酸盐在六方 In2O3 催化剂上 CO2 加氢过程中的作用

摘要 通过密度泛函理论(DFT) 计算研究了在h-In2O3(0 1 2) 和h-In2O3(1 0 4) 平面和台阶表面上CO2 加氢生成CH3OH 和CO 的完整反应途径。通过分析完整的反应途径,发现双-HCOO* 加氢为 H2COO* 是 h-In2O3(0 1 2) 平面和 h-In2O3(1 0 4) 上 CH3OH 形成的限速步骤 (RDS) ) 平坦和台阶表面,OH* 质子化为 H2O* 被确定为 h-In2O3(0 1 2) 台阶表面上 CH3OH 形成的 RDS 和 h-In2O3(0 1 2) 平坦和台阶表面上 CO 形成的 RDS表面,并且弯曲的 CO2 配置 (bt-CO2*) 质子化为 COOH* 预计是 h-In2O3(1 0 4) 平坦和台阶表面上 CO 形成的 RDS。在 h-In2O3(0 1 2) 台阶面和 h-In2O3(1 0 4) 平面和台阶面上,作为 CO2 吸附配置之一的碳酸盐(carb-CO2*)可以被视为反应过程中 Ov 位点的旁观者物种,而在 h-In2O3(0 1 2) 平面上,carb-CO2* 的质子化与 bt-CO2* 的质子化相比,对 CO 的形成贡献更大。同时,h-In2O3(0 1 2) 和 h-In2O3(1 0 4) 台阶表面上的 Ov 位点显示出比相应平坦表面更低的催化活性,因此预计它们在决定催化活性方面的作用很小。六方 In2O3 催化剂。
更新日期:2021-03-01
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