CO2 Hydrogenation to Methanol over PdZnZr Solid Solution: Effects of the PdZn Alloy and Oxygen Vacancy

被引:52
作者
Huang, Chaojie [1 ,2 ]
Wu, Zhaoxuan [1 ]
Luo, Hu [1 ]
Zhang, Shunan [1 ,2 ]
Shao, Zilong [1 ,2 ]
Wang, Hui [1 ]
Sun, Yuhan [1 ,3 ]
机构
[1] Chinese Acad Sci, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Shanghai Tech Univ, Sch Phys Sci & Technol, Shanghai 201203, Peoples R China
基金
中国国家自然科学基金;
关键词
CO2; hydrogenation; methanol; solid solution catalyst; PdZn alloy; oxygen vacancy; CATALYSTS; AROMATICS; DRIFTS; PD/ZNO; SITES; GAS; ZNO;
D O I
10.1021/acsaem.1c01502
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Utilization of CO2 with renewable hydrogen to produce value-added chemicals is highly desirable to reduce the dependence on fossil fuels. Methanol is a key intermediate for hydrocarbon products as they require a high methanol selectivity at high temperature to connect the methanol-to-olefin and methanol-to-aromatic processes. To improve the performance of CO2 hydrogenation at a higher temperature, this study prepared a 0.1% Pd/ZnZr catalyst using the coprecipitation method, which showed an 87% methanol selectivity and a space time yield of 735 g(methanol) kg(cat)(-1) h(-1) at 320 degrees C, significantly higher than that of the binary ZnZr solid solution (434 g(methanol) kg(cat)(-1) h(-1)). The characterization of the catalyst revealed that Pd2+ species formed a PdZn alloy from the ZrO2 lattice. More oxygen vacancies were generated on the surface, which enhanced the CO2 adsorption and activation capacity and then led to the formation of a higher amount of *HCOO species and better catalytic performance.
引用
收藏
页码:9258 / 9266
页数:9
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