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Elaborated Reaction Pathway of Photothermal Catalytic CO2 Conversion with H2 O on Gallium Oxide-Decorated and -Defective Surfaces.
Chemistry - A European Journal ( IF 4.3 ) Pub Date : 2022-03-28 , DOI: 10.1002/chem.202104490
Li Zhang 1 , Zheng Li 1 , Xu-Han Zhang 1 , Chen-Yu Xu 2 , Yan-Wei Zhang 1
Affiliation  

Ga2 O3 -decorated and -defective surface models based on anatase TiO2 have been established. The thermodynamic reaction pathways, including protonation, deoxygenation and hydroxylation steps, during CO2 conversion with H2 O to C1 products were calculated. The calculation results demonstrate that a Ga2 O3 cocatalyst enhances the selective adsorption of CO2 and slightly weakens the competitive adsorption of H2 O. The promotion effect of Ga2 O3 on the subsequent reaction depends on the availability of protons and electrons. Free-energy calculations revealed that the basic functional site generated by Ga2 O3 not only suppresses the back reaction of the OH group after H2 O directly provides protons but also maintains the surface defect oxygen vacancy (VO ), which promotes the reaction thermodynamics but tends to be consumed in the process. Additionally, Ga2 O3 decoration promotes VO formation, and the coexistence of Ga2 O3 and VO further decreases the reaction rate-determining step energy barrier, promoting C1 production.

中文翻译:

在氧化镓装饰和缺陷表面上与 H2 O 进行光热催化 CO2 转化的详细反应途径。

已经建立了基于锐钛矿TiO2的Ga2O3修饰和缺陷表面模型。计算了在 CO2 与 H2O 转化为 C1 产物期间的热力学反应途径,包括质子化、脱氧和羟基化步骤。计算结果表明,Ga2O3助催化剂增强了CO2的选择性吸附,略微减弱了H2O的竞争吸附。Ga2O3对后续反应的促进作用取决于质子和电子的有效性。自由能计算表明,Ga2O3 产生的基本功能位点不仅抑制了 H2O 直接提供质子后 OH 基团的逆反应,而且保持了表面缺陷氧空位(VO),这促进了反应热力学,但倾向于过程中被消耗。此外,
更新日期:2022-03-02
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