Inhibition mechanism of chlorobenzene on NH3-SCR side reactions over MnOx-CeO2 confined titania nanotubes

被引:16
作者
Li, Yifan [1 ,2 ]
Hou, Yaqin [1 ,3 ]
Li, Biao [1 ,3 ]
Yang, Yatao [1 ,2 ]
Ma, Shuang [1 ,2 ]
Wang, Bing [3 ]
Qin, Guozhen [1 ,2 ]
Huang, Zhanggen [1 ,2 ]
机构
[1] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Taiyuan Univ Technol, State Key Lab Clean & Efficient Coal Utilizat, Minist Educ, Taiyuan 030024, Peoples R China
基金
中国国家自然科学基金;
关键词
Simultaneous removal; NH3-SCR; CB oxidation; Side reactions; Inhibition mechanism; SELECTIVE CATALYTIC-REDUCTION; CHLORINATED BENZENES; NO; NH3; OXIDATION; MN; OXIDE; FE; KINETICS; GAS;
D O I
10.1016/j.fuel.2023.128619
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
The influence mechanism of CB on SCR side reactions including nonselective catalytic reduction (NSCR) and NH3 peroxidation is still a major challenge of current research. The inhibition mechanism was identified qualitatively and quantitatively on MnOx-CeO2 confined titania nanotubes catalyst with good co-remove efficiency. We decoupled NSCR into L-H and E-R mechanism routes and each mechanism were further decomposed into adsorption and reaction steps for the first time. It revealed that CB preferred to inhibit L-H mechanism (99%) and adsorption step (53.5% in E-R and 98% in L-H) in NSCR.CB dominated the inhibition of L-H mechanism and adsorption steps. As for NH3 peroxidation, N2O, NO and NO2 are produced with the increase of oxygen activity. After 240 degrees C, the inhibition of CB on N2O weakens and starts to inhibit NO and NO2 instead. It can be attributed that CB competitively reacts with higher active oxygen, weakening the oxidization of NH3 to NO/NO2. The inhibition mechanism is that the active oxygen is continuously consumed in CB oxidation process, and the dissociated Cl produced by nucleophilic substitution limits the supplement of the lattice oxygen, finally resulting in the reduction of high valence active centers and the loss of active oxygen.
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页数:11
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共 54 条
[1]   I. Adsorption mechanism of chlorophenols on iron oxides, titanium oxide and aluminum oxide as detected by infrared spectroscopy [J].
Bandara, J ;
Mielczarski, JA ;
Kiwi, J .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2001, 34 (04) :307-320
[2]   Metal oxide-confined interweaved titania nanotubes M/TNT (M = Mn, Cu, Ce, Fe, V, Cr, and Co) for the selective catalytic reduction of NOx in the presence of excess oxygen [J].
Boningari, Thirupathi ;
Pappas, Dimitrios K. ;
Smirniotis, Panagiotis G. .
JOURNAL OF CATALYSIS, 2018, 365 :320-333
[3]   Design of multi-shell Fe2O3@MnOx@CNTs for the selective catalytic reduction of NO with NH3:improvement of catalytic activity and SO2 tolerance [J].
Cai, Sixiang ;
Hu, Hang ;
Li, Hongrui ;
Shi, Liyi ;
Zhang, Dengsong .
NANOSCALE, 2016, 8 (06) :3588-3598
[4]   The activity and mechanism study of Fe-Mn-Ce/γ-Al2O3 catalyst for low temperature selective catalytic reduction of NO with NH3 [J].
Cao, Fan ;
Su, Sheng ;
Xiang, Jun ;
Wang, Pengying ;
Hu, Song ;
Sun, Lushi ;
Zhang, Anchao .
FUEL, 2015, 139 :232-239
[5]   Performance of Ce-modified V-W-Ti type catalyst on simultaneous control of NO and typical VOCS [J].
Chen, Lin ;
Liao, Yanfen ;
Chen, Yin ;
Wu, Junnan ;
Ma, Xiaoqian .
FUEL PROCESSING TECHNOLOGY, 2020, 207
[6]   Simultaneous removal of NO and volatile organic compounds (VOCs) by Ce/Mo doping-modified selective catalytic reduction (SCR) catalysts in denitrification zone of coal-fired flue gas [J].
Chen, Lin ;
Liao, Yanfen ;
Xin, Shirong ;
Song, Xinxuan ;
Liu, Guicai ;
Ma, Xiaoqian .
FUEL, 2020, 262
[7]   Remarkable N2-selectivity enhancement of practical NH3-SCR over Co0.5Mn1Fe0.25Al0.75Ox-LDO: The role of Co investigated by transient kinetic and DFT mechanistic studies [J].
Chen, Sining ;
Vasiliades, Michalis A. ;
Yan, Qinghua ;
Yang, Guangpeng ;
Du, Xuesen ;
Zhang, Cheng ;
Li, Yuran ;
Zhu, Tingyu ;
Wang, Qiang ;
Efstathiou, Angelos M. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 277
[8]   Tunning active oxygen species for boosting Hg0 removal and SO2-resistance of Mn-Fe oxides supported on (NH4)2S2O8 doping activated coke [J].
Du, Xueyu ;
Li, Caiting ;
Zhang, Jie ;
Zhu, Youcai ;
Liang, Caixia ;
Huang, Le ;
Yang, Kuang ;
Yao, Chaoliang ;
Ma, Ying .
JOURNAL OF HAZARDOUS MATERIALS, 2023, 441
[9]   Synergistic Promotion Effect between NOx and Chlorobenzene Removal on MnOx-CeO2 Catalyst [J].
Gan, Lina ;
Shi, Wenbo ;
Li, Kezhi ;
Chen, Jianjun ;
Peng, Yue ;
Li, Junhua .
ACS APPLIED MATERIALS & INTERFACES, 2018, 10 (36) :30426-30432
[10]   Adjustment of operation temperature window of Mn-Ce oxide catalyst for the selective catalytic reduction of NOx with NH3 [J].
Geng, Yang ;
Shan, Wenpo ;
Liu, Fudong ;
Yang, Shijian .
JOURNAL OF HAZARDOUS MATERIALS, 2021, 405