Reaction-driven surface reconstruction of ZnAl2O4 boosts the methanol selectivity in CO2 catalytic hydrogenation

The reaction-driven surface reconstruction of ZnAl2O4 spinel leads to the formation of amorphous ZnO, which is accompanied by the increasing catalytic activity for methanol production. [Display omitted] •The surface reconstruction of ZnAl2O4 spinel during CO2 hydrogenation was elucidated.•The reacti...

Full description

Saved in:
Bibliographic Details
Published in:Applied catalysis. B, Environmental Environmental, 2021-05, Vol.284, p.119700, Article 119700
Main Authors: Zhang, Xinbao, Zhang, Guanghui, Liu, Wei, Yuan, Fei, Wang, Jianyang, Zhu, Jie, Jiang, Xiao, Zhang, Anfeng, Ding, Fanshu, Song, Chunshan, Guo, Xinwen
Format: Article
Language:English
Subjects:
Amorphous ZnO
Carbon dioxide
Catalysts
Catalytic activity
Chemical synthesis
High temperature
Hydrogenation
Methanol
Methanol synthesis
Reconstruction
Selectivity
Surface reconstruction
Surface structure
Zinc oxide
ZnAl2O4 spinel
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:The reaction-driven surface reconstruction of ZnAl2O4 spinel leads to the formation of amorphous ZnO, which is accompanied by the increasing catalytic activity for methanol production. [Display omitted] •The surface reconstruction of ZnAl2O4 spinel during CO2 hydrogenation was elucidated.•The reaction-driven surface reconstruction of ZnAl2O4 spinel leads to the formation of amorphous ZnO in the shell.•The amorphous ZnO boosts the methanol production by promoting the activation of H2. Identifying the surface structure of heterogeneous catalysts is critical for understanding the active sites, but it remains challenging due to the difficulty in characterizing the catalytic surfaces especially at elevated temperatures. Zn-based catalysts are high-efficiency alternatives for high-temperature methanol synthesis from CO2, as well as in bifunctional catalysts for hydrocarbons synthesis. Herein, the surface reconstruction of ZnAl2O4 spinel during CO2 hydrogenation reaction was investigated using detailed spectroscopic characterization. The results indicate that the reaction-driven surface reconstruction leads to the formation of amorphous ZnO on the ZnAl2O4 surface, which is accompanied by the increasing catalytic activity for methanol production. Kinetic analysis, STEM and in situ FTIR results indicate that the amorphous ZnO boosts the methanol formation rate by promoting the activation of H2. This study provides useful insight into the structure-activity relationship of zinc-based catalysts for CO2 hydrogenation and future design of new catalysts.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2020.119700