硫黄
铂金
催化作用
密度泛函理论
金属
化学
有机化学
计算化学
作者
Xiaoyan Liu,Yiqi Ren,Maodi Wang,Xiaomin Ren,Jian Liu,Qihua Yang
出处
期刊:ACS Catalysis
[American Chemical Society]
日期:2022-09-02
卷期号:12 (18): 11369-11379
被引量:22
标识
DOI:10.1021/acscatal.2c02988
摘要
Selective hydrogenation of nitrobenzothiazole to aminobenzothiazole with metal catalysts is an economical process for the synthesis of pivotal intermediates for thiazole drugs, but it is still very difficult due to the easy deactivation of metal catalysts by sulfur-containing compounds. Herein, we report efficient nitrobenzothiazole hydrogenation using Pt/TiO2 as a catalyst. Pt/TiO2 with the strong metal–support interaction (SMSI) effect was found to be more active than Pt/TiO2 without the SMSI effect. Density functional theory (DFT) calculations and S-resistance experiments revealed that the −NO2 group is activated mainly by the oxygen vacancy (Ov) of TiOx in the presence of sulfur compounds and that H species dissociated on Pt spills over to reduce −NO2. The high nitrobenzothiazole hydrogenation activity of Pt/TiO2 can be attributed to a cooperative effect between Pt and TiOx. The generation of SMSI not only induces more Ov sites but also enhances the H-spillover capability. This study provides deep insight into the development of highly efficient platinum-S resistance hydrogenation catalysts.
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