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探究负载型 Pt 纳米和单原子催化剂上甲苯催化去除的机理。

Probing toluene catalytic removal mechanism over supported Pt nano- and single-atom-catalyst.

机构信息

Key Laboratory of Beijing on Regional Air Pollution Control, Beijing Key Laboratory for Green Catalysis and Separation, and College of Environmental and Energy Engineering, Beijing University of Technology, Beijing, 100124, China.

Guangxi Key Laboratory of Agricultural Resources Chemistry and Biotechnology, College of Chemistry and Food Science, Yulin Normal University, Yulin, 537000, Guangxi, China.

出版信息

J Hazard Mater. 2020 Jun 15;392:122258. doi: 10.1016/j.jhazmat.2020.122258. Epub 2020 Feb 13.

DOI:10.1016/j.jhazmat.2020.122258
PMID:32092645
Abstract

Commercial TiO supported 0.20 wt% Pt catalyst is obtained via the molten salt method, and both Pt nanoparticles and single atom Pt sites are observed. It exhibits high catalytic performance for toluene oxidation, with T and T being 173 and 183 °C, respectively. Reaction intermediates including benzene, p-xylene, o-xylene, benzaldehyde, phthalic acid, maleic anhydride, itaconic anhydride, acetone, and acetic acid, are detected during toluene oxidation. On this basis, likely toluene combustion reaction pathway is provided. Benzaldehyde is the most stable surface intermediate, and its oxidation can be rate-limiting for the entire toluene oxidation reaction. 2-10.0 vol% HO slightly inhibits the reaction by competing surface sites with the reactant, while it does not poison the catalyst. 2.5-10.0 vol% CO slightly poisons the catalyst by surface carbonate formation, whereas 50 ppm SO severely poisons the catalyst by sulfite/sulfate formation.

摘要

商业 TiO 负载的 0.20wt%Pt 催化剂通过熔融盐法获得,观察到 Pt 纳米颗粒和单原子 Pt 位。它对甲苯氧化表现出高催化性能,T 和 T 分别为 173 和 183°C。在甲苯氧化过程中检测到包括苯、对二甲苯、邻二甲苯、苯甲醛、邻苯二甲酸、马来酸酐、衣康酸酐、丙酮和乙酸在内的反应中间体。在此基础上,提供了可能的甲苯燃烧反应途径。苯甲醛是最稳定的表面中间体,其氧化可能是整个甲苯氧化反应的速率限制步骤。2-10.0 体积%HO 通过与反应物竞争表面位稍微抑制反应,而不会使催化剂中毒。2.5-10.0 体积%CO 通过表面碳酸盐形成轻微使催化剂中毒,而 50ppm SO 通过亚硫酸盐/硫酸盐形成严重使催化剂中毒。

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