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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H2O和CO2对活性位点受Lewis酸度调控的Pt/SSZ-13上CO氧化的影响

利用沸石控制金属形态大小的策略及其在工业相关过程中的催化行为已引起广泛关注，但H2O和CO2对沸石基金属催化剂催化性能的影响尚不清楚。本研究考察了H2O和CO2对沸石基金属催化剂上CO氧化的影响，以及通过调节Lewis酸度对活性位点的精确控制。结果表明，H2O的存在增强了CO的氧化作用，减轻了CO2的抑制作用。Pt/SSZ-13催化剂中大量的低SiO2/Al2O3比的Lewis酸位点有利于Pt的分散（61.07%）、高Ptn+/Pt比（4.43）和小Pt颗粒（2.31 nm）的形成。原位漂移表明，CO2抑制CO吸附和碳中间体的分解。水改变了Pt0对CO的吸附构型，从而削弱了Pt-CO键，促进了CO氧化反应。同时，表面解离成羟基的水吸附氧，参与反应，促进碳中间体产生CO2。H218O同位素标记实验验证了水参与反应，并强调了水解离过程中氧存在的重要性。Lewis酸位点的调控促进了Ptn+的形成，增强了CO氧化活性，而Pt0则增强了促水作用。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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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.