Engineering Interfacial Oxygen Vacancies of Zn–Cr Sites for CO2 Activation and Hydrogenation

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-04-18 DOI:10.1021/acscatal.5c00766

Jiaming Liang, Lei Jiang, Hengyang Liu, Bowei Meng, Zhiliang Jin, Lisheng Guo, Zhihao Liu, Teng Li, Wenhang Wang, Chengwei Wang, Ying Shi, Guangbo Liu, Kai Sun, Yingluo He, Bing Liang, Noritatsu Tsubaki

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引用次数: 0

Abstract

Understanding the influence of oxygen vacancies is of great significance for revealing molecular adsorption and rational catalyst design. However, for the catalysts with multiple phases, the properties and intrinsic catalytic mechanism of oxygen vacancies on varied active sites have not been studied thoroughly. Herein, Zn–Cr catalysts with different oxygen vacancy distributions and contents are synthesized by engineering interfacial oxygen vacancies for CO₂ hydrogenation. Characterization and DFT calculations illustrate that although the oxygen vacancies are not prone to being generated on the monointerface between ZnO and ZnCr₂O₄ compared with the spinel or metal oxide phases, the ZnO/ZnCr₂O₄–O_v interfacial oxygen vacancy sites reduce the energy barriers of crucial HCOO* and H₃CO* intermediate formation for CH₃OH synthesis. With the assistance of the well-dispersed interface oxygen vacancies, 3Zn1Cr displays the highest methanol selectivity (80.5%) as well as the highest CO₂ conversion (19.2%) among all of the ratios of Zn–Cr catalysts. After further combination of 3Zn1Cr with modified β zeolite, the composite catalyst showed a superior liquefied petroleum gas selectivity of 84.0% at a CO₂ conversion of 30.2%. The proposed strategy here sheds light on the efficient composite catalyst design via a methanol-mediated route for C1 chemistry.

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.