Improving methanol selectivity in CO2 hydrogenation by tuning the distance of Cu on catalyst

被引：55

作者：

Cui, Xiaojing ^{[1
]}

Chen, Shuai ^{[2
]}

Yang, Huanhuan ^{[3
]}

Liu, Yequn ^{[2
]}

Wang, Huifang ^{[1
]}

Zhang, He ^{[1
]}

Xue, Yanfeng ^{[1
]}

Wang, Guofu ^{[2
]}

Niu, Yulan ^{[1
]}

Deng, Tiansheng ^{[2
]}

Fan, Weibin ^{[2
]}

机构：

[1] Taiyuan Inst Technol, Inst Interface Chem & Engn, Dept Chem & Chem Engn, 31 Xinlan Rd, Taiyuan 030008, Peoples R China

[2] Chinese Acad Sci, Inst Coal Chem, 27 South Taoyuan Rd, Taiyuan 030001, Peoples R China

[3] Zhengzhou Univ, Henan Inst Adv Technol, 97 Wenhua Rd, Zhengzhou 450003, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2021年 / 298卷

基金：

中国国家自然科学基金;

关键词：

CO2; hydrogenation; Methanol; Cu/ZnO catalyst; Distance effect; Hydrogen spillover; HYDROTALCITE-LIKE PRECURSORS; ZINC-OXIDE; CU/ZN/AL/ZR CATALYSTS; ACTIVE-SITES; COPPER; SPILLOVER; WATER; ZNO; SYNERGY; PD;

D O I：

10.1016/j.apcatb.2021.120590

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：

It is desirable but challenging to obtain high methanol selectivity in CO2 hydrogenation on Cu/ZnO catalysts. Herein, we dispersed a commercial Cu/ZnO/Al2O3 on a silica support for CO2 hydrogenation to methanol, and discovered by high-angle annular dark-field scanning transmission electron microscopy (HADDF-STEM) that the distance between Cu nanoparticles on silica tuned the total methanol selectivity from 35.5 mol% to 88.9 mol%. This distance effect of Cu was elucidated by H-2-TPR, FT-IR, in situ DRIFT, and catalyst silylation modification. It was identified that the active hydrogen species produced on Cu diffuse onto silica via the surface silanols, promoting reverse water gas shift (RWGS) reaction to produce CO. The average concentration of spilled hydrogen species was decreased along with the distance of Cu on silica, suppressing RWGS reaction and thus highlighting methanol selectivity. We anticipate that the distance effect observed here is prevalent on metal supported catalysts in other (de)hydrogenation reactions.

引用

页数：11

共 46 条

[21] CATALYSIS Active sites for CO2 hydrogenation to methanol on Cu/ZnO catalysts [J].