A first-principles study of reaction mechanism over carbon decorated oxygen-deficient TiO2 supported Pd catalyst in direct synthesis of H2O2

被引：12

作者：

Yao, Zihao ^{[1
]}

Zhao, Jinyan ^{[1
]}

Zhao, Chenxia ^{[1
]}

Deng, Shengwei ^{[1
]}

Zhuang, Guilin ^{[1
]}

Zhong, Xing ^{[1
]}

Wei, Zhongzhe ^{[1
]}

Li, Yang ^{[1
]}

Wang, Shibin ^{[1
]}

Wang, Jianguo ^{[1
]}

机构：

[1] Zhejiang Univ Technol, Coll Chem Engn, Inst Ind Catalysis, Hangzhou 310032, Peoples R China

来源：

CHINESE JOURNAL OF CHEMICAL ENGINEERING | 2021年 / 31卷

基金：

中国国家自然科学基金;

关键词：

Direct synthesis of H2O2; DFT; Supported Pd-catalysts; TiO2-support; Carbon-doped; Oxygen vacancies; DENSITY-FUNCTIONAL THEORY; FISCHER-TROPSCH SYNTHESIS; WASTE-WATER TREATMENT; HYDROGEN-PEROXIDE; METAL-SUPPORT; QUANTITATIVE-DETERMINATION; ELECTRONIC-PROPERTIES; PD/TIO2; CATALYSTS; CO OXIDATION; SELECTIVITY;

D O I：

10.1016/j.cjche.2020.11.016

中图分类号：

TQ [化学工业];

学科分类号：

0817 ;

摘要：

The choice of support is one of the most significant components in the direct synthesis of H2O2. Aiming to improvement of activity and selectivity of H2O2 on Pd/TiO2 surface, we systematically investigated the important elementary steps on Pd/TiO2-Vo@C, Pd/TiO2-Vo, Pd/TiO2-2Vo, Pd/TiO2, and Pd/C using the first-principles calculations. The Bader charge analysis and charge density difference of O-2 adsorption elucidate the relationship between the electronic distribution and chemisorption energy. The effective barrier analysis further enables to quantitatively estimate the reactivity of H2O2 and H2O. We demonstrate unambiguously that the selectivity of H2O formation is boosted as the oxygen vacancy concentration raised. Moreover, the introduction of C into a TiO2 with appropriate oxygen vacancies can slightly reduce the effective barrier for H2O2 formation and increase the effective barrier for H2O formation leading to a higher activity and selectivity of H2O2 formation. Our finding suggests that carbon-doped oxygen vacancy TiO2 supported Pd is potential alternative catalyst compared with the Pd/TiO2. (C) 2020 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.

引用

页码：126 / 134

页数：9

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