Experimental and theoretical studies of carbon monoxide oxidation over W/Cu/Ce trimetallic oxides: the effect of W addition

• Published in: Materials today chemistry 2023-01, Vol.27, p.101295, Article 101295
• Main Authors: Huang, Mingzhen, Hu, Siyuan, Cai, Dongren, Zhan, Guowu
• Format: Article
• Language: English
• Subjects: CO oxidation; DFT calculation; In-situ DRIFTS; W(x)/Cu/CeO2
• ISSN: 2468-5194; 2468-5194
• DOI: 10.1016/j.mtchem.2022.101295

It is a significant method to prepare highly dispersed polymetallic oxides using in-situ doping metal organic frameworks as precursors. Herein, a series of straw-like W/Cu/Ce trimetallic oxides were prepared by using phosphotungstic ionic liquid@Ce-based metal organic framework adsorbing with copper acetylacetonate as precursors. The effect of W content on catalytic activity of W/Cu/Ce trimetallic oxides for carbon monoxide (CO) oxidation was well-investigated. Comprehensive characterization methods and density functional theory calculations were adopted to reveal the property changes of Cu/CeO2 catalyst by the addition of W. The results demonstrated that W, Cu, and Ce are highly dispersed in the prepared W/Cu/Ce trimetallic oxides, and adding proper amount of W can improve the activity of the catalyst. H2 temperature-program reduction profiles, X-ray photoelectron spectroscopy, in-situ diffuse reflectance infrared Fourier transform spectroscopy, and density functional theory calculations clearly revealed that after the addition of W, the strength of Ce-O bond is weakened, the oxygen vacancy is increased, and the adsorption of CO is enhanced, respectively, which are vital reasons for its high catalytic activity. In addition, the CO oxidation reaction pathway over prepared W/Cu/Ce trimetallic oxides based on the Mars-van Krevelen mechanism was studied, and the results exhibited that CO can wrest the lattice oxygen of W/Cu/Ce trimetallic oxides to form CO2, which is also proved to be the rate-determining step in reaction process. •W/Cu/Ce oxides with high dispersion and tailorable compositions were prepared.•The prepared W/Cu/Ce oxides exhibited high activity and stability in CO oxidation.•In-situ DRIFTS was used to study CO oxidation process over W/Cu/Ce oxides.•DFT was used to simulate the CO oxidation process over W/Cu/Ce oxides.