Unlocking the positive effect of non-polar ZnO facets in ZrZnOx catalysts for CO2 hydrogenation

IF 3.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis Pub Date : 2025-03-28 DOI:10.1016/j.mcat.2025.115059

Xiaohong Guo, Liqiang Deng, Xiaoyue Wang, Yongjie Zhao, Zhifan Cao, Pengwei Li, Congming Li

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Abstract

A pivotal aspect in advancing ZrZnO_x catalysts for CO₂ hydrogenation lies in the modulation of Zr-O-Zn active sites, with ZnO facets emerging as potential modulators of site activity. Whereas the beneficial influence of non-polar ZnO facets on ZrZnO_x catalysts has been scarcely documented. Our investigation reveals that ZrZnO_x catalysts exposed non-polar ZnO facets (ZrZnO-n) exhibit superior methanol selectivity (74 %) compared to those with randomly exposed ZnO facets (ZrZnO-r, 35 %). Characterization results demonstrate that it is ascribed to the formation of highly active Zr-O-Zn^(2−δ)+ sites on ZrZnO-n, which facilitate H₂ adsorption and dissociation. In situ spectroscopic studies and DFT calculations further substantiate this finding, demonstrating enhanced intermediates formation and more efficient hydrogenation processes. This research underscores the significance of ZnO facet engineering in the purposeful creation of efficient ZrZnO_x catalysts for CO₂ hydrogenation.

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来源期刊

Molecular Catalysis Chemical Engineering-Process Chemistry and Technology

CiteScore

6.90

自引率

10.90%

发文量

700

审稿时长

40 days

期刊介绍： Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods