Interaction Mechanism for Simultaneous Elimination of Nitrogen Oxides and Toluene over the Bifunctional CeO2-TiO2 Mixed Oxide Catalyst

被引:84
作者
Liu, Hao [1 ]
Chen, Jianjun [1 ]
Wang, Ya [1 ]
Yin, Rongqiang [1 ]
Yang, Wenhao [1 ]
Wang, Guimin [1 ]
Si, Wenzhe [1 ]
Peng, Yue [1 ]
Li, Junhua [1 ]
机构
[1] Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China
基金
中国国家自然科学基金;
关键词
CeO2-TiO2 mixed oxide; NH3-SCR; toluene oxidation; multipollutant co-control; reaction mechanism; NH3-SCR REACTION; REDUCTION; OXIDATION; PERFORMANCE; NOX; PROPENE; NANOPARTICLES; SPECTROSCOPY; ETHANOL; NH3;
D O I
10.1021/acs.est.1c08424
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Simultaneous catalytic elimination of nitrogen oxides (NOx, x = 1 and 2) and volatile organic compounds (VOCs) is of great importance for environmental preservation in China. In this work, the interactions of simultaneous removal of NOx and methylbenzene (PhCH3) were investigated on a CeO2-TiO2 mixed oxide catalyst, which demonstrated excellent bifunctional removal efficiencies for the two pollutants. The results indicated that NOx positively promotes PhCH3 oxidation, while NH3 negatively inhibits through competitive adsorption with PhCH3. The underlying mechanism is that a pseudo PhCH3-SCR reaction happened in this process is parallel to NH3-SCR. Combined with in situ diffuse reflectance infrared Fourier transform spectroscopy and quasi in situ X-ray photoelectron spectroscopy, the interaction mechanism between NOx and PhCH3 is proposed. Specifically, NOx is adsorbed on the catalyst surface to produce nitrate species, which reacts with the carboxylate generated during PhCH3 oxidation to form organic nitrogen intermediates that create N-2 and CO2 in the following reactions. In the reaction process, the superoxide (O-2(-)) generated by O-2 activation on the catalyst surface is an important species for the propelling of oxidation reaction. This work could provide guidelines for the design of state-of-the-art catalysts for simultaneous catalytic removal of NOx and VOCs.
引用
收藏
页码:4467 / 4476
页数:10
相关论文
共 50 条
[1]   Enhancing the Catalytic Activity of Palladium Nanoparticles via Sandwich-Like Confinement by Thin Titanate Nanosheets [J].
Ament, Kevin ;
Wagner, Daniel R. ;
Goetsch, Thomas ;
Kikuchi, Takayuki ;
Kroehnert, Jutta ;
Trunschke, Annette ;
Lunkenbein, Thomas ;
Sasaki, Takayoshi ;
Breu, Josef .
ACS CATALYSIS, 2021, 11 (05) :2754-2762
[2]   Effect of Formaldehyde in Selective Catalytic Reduction of NOx by Ammonia (NH3-SCR) on a Commercial V2O5-WO3/TiO2 Catalyst under Model Conditions [J].
Anh Binh Ngo ;
Thanh Huyen Vuong ;
Atia, Hanan ;
Bentrup, Ursula ;
Kondratenko, Vita A. ;
Kondratenko, Evgenii V. ;
Rabeah, Jabor ;
Ambruster, Udo ;
Bruckner, Angelika .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2020, 54 (19) :11753-11761
[3]   Cr-MnOx mixed-oxide catalysts for selective catalytic reduction of NOx with NH3 at low temperature [J].
Chen, Zhihang ;
Yang, Qing ;
Li, Hua ;
Li, Xuehui ;
Wang, Lefu ;
Tsang, Shik Chi .
JOURNAL OF CATALYSIS, 2010, 276 (01) :56-65
[4]   Revealing the Highly Catalytic Performance of Spinel CoMn2O4 for Toluene Oxidation: Involvement and Replenishment of Oxygen Species Using In Situ Designed-TP Techniques [J].
Dong, Cui ;
Qu, Zhenping ;
Qin, Yuan ;
Fu, Qiang ;
Sun, Hongchun ;
Duan, Xiaoxiao .
ACS CATALYSIS, 2019, 9 (08) :6698-6710
[5]   Electron donation of non-oxide supports boosts O2 activation on nano-platinum catalysts [J].
Gan, Tao ;
Yang, Jingxiu ;
Morris, David ;
Chu, Xuefeng ;
Zhang, Peng ;
Zhang, Wenxiang ;
Zou, Yongcun ;
Yan, Wenfu ;
Wei, Su-Huai ;
Liu, Gang .
NATURE COMMUNICATIONS, 2021, 12 (01)
[6]   Recent advances in VOC elimination by catalytic oxidation technology onto various nanoparticles catalysts: a critical review [J].
Guo, Yunlong ;
Wen, Meicheng ;
Li, Guiying ;
An, Taicheng .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2021, 281
[7]   Selective Catalytic Reduction of NOx with NH3 by Using Novel Catalysts: State of the Art and Future Prospects [J].
Han, Lupeng ;
Cai, Sixiang ;
Gao, Min ;
Hasegawa, Jun-ya ;
Wang, Penglu ;
Zhang, Jianping ;
Shi, Liyi ;
Zhang, Dengsong .
CHEMICAL REVIEWS, 2019, 119 (19) :10916-10976
[8]   Role of surface peroxo and superoxo species in the low-temperature oxygen buffering of ceria: Density functional theory calculations [J].
Huang, Min ;
Fabris, Stefano .
PHYSICAL REVIEW B, 2007, 75 (08)
[9]   Regulating oxygen activity of perovskites to promote NOx oxidation and reduction kinetics [J].
Hwang, Jonathan ;
Rao, Reshma R. ;
Giordano, Livia ;
Akkiraju, Karthik ;
Wang, Xiao Renshaw ;
Crumlin, Ethan J. ;
Bluhm, Hendrik ;
Shao-Horn, Yang .
NATURE CATALYSIS, 2021, 4 (08) :663-673
[10]   Synergistic Elimination of NOx and Chloroaromatics on a Commercial V2O5-WO3/TiO2 Catalyst: Byproduct Analyses and the SO2 Effect [J].
Jiang, Weiyu ;
Yu, Yulei ;
Bi, Feng ;
Sun, Pengfei ;
Weng, Xiaole ;
Wu, Zhongbiao .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2019, 53 (21) :12657-12667