Activating low-temperature NH3-SCR catalyst by breaking the strong interface between acid and redox sites: A case of model Ce2(SO4)3-CeO2 study

被引：80

作者：

Ji, Jiawei ^{[1
]}

Jing, Meizan ^{[4
]}

Wang, Xiuwen ^{[1
]}

Tan, Wei ^{[1
]}

Guo, Kai ^{[1
]}

Li, Lulu ^{[3
,5
]}

Wang, Xin ^{[1
]}

Song, Wang ^{[1
]}

Cheng, Lijun ^{[3
]}

Sun, Jingfang ^{[1
,2
]}

Song, Weiyu ^{[4
]}

Tang, Changjin ^{[1
,2
,3
]}

Liu, Jian ^{[4
]}

Dong, Lin ^{[1
,2
]}

机构：

[1] Nanjing Univ, Sch Chem & Chem Engn, Lab Mesoscop Chem MOE, Nanjing 210023, Peoples R China

[2] Nanjing Univ, Sch Environm, Ctr Modern Anal, Jiangsu Key Lab Vehicle Emiss Control, Nanjing 210023, Peoples R China

[3] Nanjing Normal Univ, Sch Environm, Nanjing 210023, Peoples R China

[4] China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China

[5] Jiangsu Univ Sci & Technol, Sch Environm & Chem Engn, Zhenjiang 212003, Jiangsu, Peoples R China

来源：

JOURNAL OF CATALYSIS | 2021年 / 399卷

基金：

中国国家自然科学基金;

关键词：

NH3-SCR; Ce-2(SO4)(3); CeO2; Acid/redox sites; Interfacial interaction; TOTAL-ENERGY CALCULATIONS; REACTION-MECHANISM; SELECTIVE REDUCTION; GETTING INSIGHT; NO; CEO2; NH3; PERFORMANCE; VANADIA; SO2;

D O I：

10.1016/j.jcat.2021.05.001

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Y The occurrence of NH3-SCR (selective catalytic reduction of NO with NH3) reaction on catalyst surface typically requires acid and redox sites. However, the role of acid-redox interaction on NH3-SCR performance is still obscure due to complex acidities and entangled acid-redox sites. Herein, three types of model Ce-2(SO4)(3)-CeO2 catalysts with distinct interfaces are constructed to reveal the effect of acidredox interaction on NH3-SCR performance. That is, SO42-/CeO2-VS (vapor sulfation of ceria) with strong acid-redox interfacial contact, SO42-/CeO2-WI (wet impregnation), and SO42-/CeO2-SG (solid grinding) with limited interfaces. It is found the redox property is significantly disturbed as a result of the electronwithdrawing effect from the sulfate. Theoretical result unravels that the introduction of Ce-2(SO4) (3) retards the oxygen vacancy formation over CeO2. Due to restricted interfaces in SO42-/CeO2-SG, the negative influence from acid sites is greatly alleviated. Further mechanism study discloses the weakened acid-redox interaction actually changes the nature of surface NOx species, resulting in the generation of reactive species (*O-N-O* and cis-N2O22-) and the promotion of surface reaction via Langmuir-Hinshelwood (L-H) mechanism. (C) 2021 Elsevier Inc. All rights reserved.

引用

页码：212 / 223

页数：12

共 58 条

[1] A complete reaction mechanism for standard and fast selective catalytic reduction of nitrogen oxides on low coverage VOx/TiO2(001) catalysts [J].

Arnarson, Logi ;

Falsig, Hanne ;

Rasmussen, Soren B. ;

Lauritsen, Jeppe V. ;

Moses, Poul Georg .

JOURNAL OF CATALYSIS, 2017, 346 :188-197

[2] PROJECTOR AUGMENTED-WAVE METHOD [J].

BLOCHL, PE .

PHYSICAL REVIEW B, 1994, 50 (24) :17953-17979

[3] Chemical and mechanistic aspects of the selective catalytic reduction of NOx by ammonia over oxide catalysts:: A review [J].

Busca, G ;

Lietti, L ;

Ramis, G ;

Berti, F .

APPLIED CATALYSIS B-ENVIRONMENTAL, 1998, 18 (1-2) :1-36

[4] Migration of cations and shell functionalization for Cu-Ce-La/SSZ-13@ZSM-5: The contribution to activity and hydrothermal stability in the selective catalytic reduction reaction [J].

Chen, Zhiqiang ;

Liu, Li ;

Qu, Hongxia ;

Zhou, Baojing ;

Xie, Huifang ;

Zhong, Qin .

JOURNAL OF CATALYSIS, 2020, 392 :217-230

[5] Linear response approach to the calculation of the effective interaction parameters in the LDA+U method [J].

Cococcioni, M ;

de Gironcoli, S .

PHYSICAL REVIEW B, 2005, 71 (03)

[6] Revisiting effects of alkali metal and alkaline earth co-cation additives to Cu/SSZ-13 selective catalytic reduction catalysts [J].

Cui, Yanran ;

Wang, Yilin ;

Mei, Donghai ;

Walter, Eric D. ;

Washton, Nancy M. ;

Holladay, Jamie D. ;

Wang, Yong ;

Szanyi, Janos ;

Peden, Charles H. F. ;

Gao, Feng .

JOURNAL OF CATALYSIS, 2019, 378 :363-375

[7] Reply to "Comment on 'Taming multiple valency with density functionals: A case study of defective ceria'" [J].

Fabris, S ;

de Gironcoli, S ;

Baroni, S ;

Vicario, G ;

Balducci, G .

PHYSICAL REVIEW B, 2005, 72 (23)

[8] Development of stable and efficient CeVO4 systems for the selective reduction of NOx by ammonia: Structure-activity relationship [J].

Gillot, Sylvain ;

Tricot, Gregory ;

Vezin, Herve ;

Dacquin, Jean-Philippe ;

Dujardin, Christophe ;

Granger, Pascal .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 218 :338-348

[9] What News in the Surface Chemistry of Bulk and Supported Vanadia Based SCR-Catalysts: Improvements in their Resistance to Poisoning and Thermal Sintering [J].

Granger, Pascal ;

Siaka, Hermann W. ;

Umbarkar, Shubhangi B. .

CHEMICAL RECORD, 2019, 19 (09) :1813-1828

[10] Identification of neutral and charged NxOy surface species by IR spectroscopy [J].

Hadjiivanov, KI .

CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 2000, 42 (1-2) :71-144

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