Effect of H2O and CO2 on CO oxidation over Pt/SSZ-13 with active sites regulated by Lewis acidity.

IF 3.1 2区化学 Q3 CHEMISTRY, PHYSICAL

Journal of Chemical Physics Pub Date : 2024-12-21 DOI:10.1063/5.0242302

Yunhe Li, Yanming Ma, Yilin Wei, Peiyuan Liang, Yixuan Yu, Wei Pei, Tianjun Sun

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引用次数: 0

Abstract

Strategies for controlling the size of metal species using zeolites and their catalytic behavior in industrially relevant processes have attracted widespread attention, but the effect of H2O and CO2 on the catalytic performance of zeolite-based metal catalysts remains obscure. This study investigated the influence of H2O and CO2 on CO oxidation over zeolite-based metal catalysts, along with the precise control of active sites through the regulation of Lewis acidity. It was found that the presence of H2O enhanced CO oxidation and alleviated the inhibitory effect of CO2. Abundant Lewis acid sites of low SiO2/Al2O3 ratios in the Pt/SSZ-13 catalyst facilitate Pt dispersion (61.07%), a high Ptn+/Pt ratio (4.43), and small Pt particles (2.31 nm) formation. In situ DRIFTS revealed that CO2 inhibits CO adsorption and the decomposition of carbon intermediates. Water alters the CO adsorption configuration of Pt0, thereby weakening the Pt-CO bond to promote the CO oxidation reaction. Meanwhile, water dissociated into hydroxyl groups on the surface adsorbs oxygen species, participating in reactions and promoting CO2 production from carbon intermediates. H218O isotope labeling experiments validated the water involvement in the reaction and emphasized the importance of the presence of oxygen species during the water dissociation process. Regulation of Lewis acid sites promotes the Ptn+ species formation, enhancing the CO oxidation activity, while Pt0 species enhance the water-promotion effect.

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来源期刊

Journal of Chemical Physics 物理-物理：原子、分子和化学物理

CiteScore

7.40

自引率

15.90%

发文量

1615

审稿时长

2 months

期刊介绍： The Journal of Chemical Physics publishes quantitative and rigorous science of long-lasting value in methods and applications of chemical physics. The Journal also publishes brief Communications of significant new findings, Perspectives on the latest advances in the field, and Special Topic issues. The Journal focuses on innovative research in experimental and theoretical areas of chemical physics, including spectroscopy, dynamics, kinetics, statistical mechanics, and quantum mechanics. In addition, topical areas such as polymers, soft matter, materials, surfaces/interfaces, and systems of biological relevance are of increasing importance. Topical coverage includes: Theoretical Methods and Algorithms Advanced Experimental Techniques Atoms, Molecules, and Clusters Liquids, Glasses, and Crystals Surfaces, Interfaces, and Materials Polymers and Soft Matter Biological Molecules and Networks.