Engineering the Nucleophilic Active Oxygen Species in CuTiOx for Efficient Low-Temperature Propene Combustion

被引:72
作者
Fang, Yarong [1 ]
Li, Li [1 ]
Yang, Ji [1 ]
Hoang, Son [1 ]
Wang, Liming [2 ]
Xu, Jue [1 ]
Yang, Weiwei [1 ]
Pan, Chuanqi [1 ]
Zhu, Yuhua [1 ]
Deng, Hongtao [1 ]
Luo, Zhu [1 ]
Sun, Chuanzhi [3 ]
Gao, Daqiang [4 ]
Li, Zhenguo [5 ]
Guo, Yanbing [1 ]
机构
[1] Cent China Normal Univ, Coll Chem, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol,Minist Educ, Wuhan 430079, Peoples R China
[2] Chinese Acad Sci, Inst High Energy Phys, CAS Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China
[3] Shandong Normal Univ, Coll Chem Chem Engn & Mat Sci, Inst Mat & Clean Energy, Shandong Prov Key Lab Clean Prod Fine Chem, Jinan 250014, Peoples R China
[4] Lanzhou Univ, Key Lab Magnetism & Magnet Mat, Key Lab Special Funct Mat & Struct Design, MOE, Lanzhou 730000, Gansu, Peoples R China
[5] China Automot Technol & Res Ctr Co Ltd, Natl Engn Lab Mobile Source Emiss Control Technol, Tianjin 300300, Peoples R China
基金
中国国家自然科学基金;
关键词
C3H6; combustion; Cu-O-Ti hybridization; nucleophilic O; H abstraction; PROPYLENE PARTIAL OXIDATION; VOLATILE ORGANIC-COMPOUNDS; CATALYTIC-OXIDATION; OZONE FORMATION; MIXED OXIDES; CO; TIO2; CU; EPOXIDATION; ADSORPTION;
D O I
10.1021/acs.est.0c05845
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Industrialization has resulted in the rapid increase of volatile organic compound (VOC) emissions, which have caused serious issues to human health and the environment. In this study, an extensive Cu incorporating TiO2 induced nucleophilic oxygen structure was constructed in the CuTiOx catalyst, which exhibited superior low-temperature catalytic activity for C3H6 combustion. Thorough structural, surface characterization and density functional theory (DFT) calculations revealed that the Cu-O-Ti hybridization induced nucleophilic oxygen initiates C3H6 combustion by abstracting the C-H bond. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results indicated that incorporated copper species acted as the major adsorbent site for the propene molecule. In combination of the DRIFTS and DFT results, the promotion effect of the nucleophilic O on the C-H bond abstraction and CO2 formation pathway was proposed. The surface doping induced nucleophilic oxygen as strong Bronsted basic sites for low-temperature propene combustion exemplified an efficient strategy for rational design of next-generation environmental catalysts.
引用
收藏
页码:15476 / 15488
页数:13
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