文献类型：期刊文献

英文题名：Catalytic oxidation of propane over nanorod-like TiO2 supported Ru catalysts: Structure-activity dependence and mechanistic insights

作者：Wang, Mingju[1];Li, Guanghao[1];Wang, Shijie[1];Liu, Xuehua[1];Wang, Aiyong[2];Cao, Haijie[1];Zhang, Chuanhui[1]

机构：[1]Qingdao Univ, Inst Mat Energy & Environm, Coll Mat Sci & Engn, Qingdao 266071, Peoples R China;[2]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, Shanghai 200237, Peoples R China

年份：2024

卷号：481

外文期刊名：CHEMICAL ENGINEERING JOURNAL

收录：;EI(收录号：20240215348052);WOS:【SCI-EXPANDED(收录号:WOS:001153201500001)】；

基金：This work was financially supported by the National Natural Science Foundation of China (No. 22076088) , the Natural Science Foundation of Shandong province (No. ZR2023QB061) , Qingdao New Energy Shan- dong Laboratory Open Project (No. QNESLOP202310) and Key Research Project of Zibo (Integration with external universities, No. 2021XCYF0035) .

语种：英文

外文关键词：Nanorod-likeTiO(2); Catalytic oxidation; Metal-support interaction; Surface lattice oxygen; Reaction mechanism

摘要：Nanorod-like titanium dioxide (TiO2-Rod) supported ruthenium catalysts with variable metal loadings (designated as x-Ru/TiO2-Rod, x = 0.1, 0.5, 1.0 and 1.5 wt.%) were prepared for the catalytic oxidation of propane. The unique nanorod-like structure and high specific surface area of TiO2-Rod support was favorable for the surface distribution of ruthenium nanoparticles, constructing highly active redox sites for propane oxidation. Light-off experimental results indicated that the x-Ru/TiO2-Rod catalysts exhibited diverse catalytic activities for propane oxidation, giving a volcanic sequence of 0.1-Ru/TiO2-Rod < 0.5-Ru/TiO2-Rod < 1.5-Ru/TiO2-Rod < 1.0-Ru/TiO2-Rod with the increasing ruthenium content. Additionally, the optimal 1.0-Ru/TiO2-Rod delivered adequate catalytic stability and CO2/water resistant ability under complex industrial conditions. Characterization results revealed that the metallic Ru-0 and the surface lattice oxygen species from the Ru-TiO(2 )interface were demonstrated to be the catalytic active components, which played an essential role in the reaction. In situ DRIFTs analysis verified the formation of acetate, acetone and formate species as the predominant organic intermediates in propane oxidation, which may result from two plausible reaction pathways depending on the activation of terminal methyl group (-CH3) and the central methylene (CH2) group in propane molecule. This work provides fundamental guidance for the development of Ru-based catalysts and the reaction mechanism understanding for light alkanes oxidation.