Crystal Phase-Dependent Dispersion and Catalysis of the Ag Species Supported on TiO2 for CO Oxidation with Excess Oxygen

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-01-29 DOI:10.1021/acscatal.4c07381

Cen Tang, Qiuyu Huang, Ziwei Wang, Yongfang Sun, Jieqiong Ding, Fei Wang, Weixin Huang, Xiaodong Wen, Zhenhua Zhang

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Abstract

Oxidation-induced dispersion of supported metal catalysts has been frequently observed in gas–solid heterogeneous reactions, while precise tailoring of the structures of restructured metals remains challenging. Here, we successfully demonstrated the feasibility of using different TiO₂ crystal phases to tune the nanostructures of restructured silver species upon CO oxidation with excess O₂. Compared to pure anatase and rutile phases, a mixture of anatase and rutile phases (m-TiO₂) is more advantageous for the dispersion of supported Ag species, with a particle size distribution of 3.5 ± 0.2 nm, which is closely related to the surface OH group and defect concentrations of TiO₂ supports. Spectroscopic characterizations clearly reveal the CO oxidation catalyzed by the Ag/TiO₂ catalysts following a Mars–van Krevelen mechanism. Consequently, in addition to the Ag dispersion, a Ag/m-TiO₂ catalyst with higher active oxygen species contents and correspondingly better reducibility, relevant for CO activation and reactivity, contributes to better catalytic performance in CO oxidation. These results highlight the potential of crystal phases of oxide supports in tailoring oxidation-induced restructuring to develop efficient heterogeneous catalysts for applications.

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在过量氧气的 CO 氧化过程中，TiO2 上支持的 Ag 物种的晶相依赖性分散和催化作用

在气固非均相反应中经常观察到负载型金属催化剂的氧化诱导分散，而精确调整重组金属的结构仍然具有挑战性。在这里，我们成功地证明了使用不同的TiO2晶体相来调整CO与过量O2氧化后重组银的纳米结构的可行性。与纯锐钛矿和金红石相相比，锐钛矿和金红石相的混合物（m-TiO2）更有利于负载Ag的分散，粒径分布为3.5±0.2 nm，这与TiO2载体表面OH基团和缺陷浓度密切相关。光谱表征清楚地揭示了Ag/TiO2催化剂催化CO氧化遵循Mars-van Krevelen机制。因此，除了Ag的分散性外，与CO活化和反应性相关的较高的活性氧含量和相应的更好的还原性的Ag/m-TiO2催化剂有助于更好的CO氧化催化性能。这些结果突出了氧化载体的晶体相在调整氧化诱导重组方面的潜力，从而开发出高效的非均相催化剂。

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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.