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

被引：89

作者：

Chen, Sining ^{[1
]}

Vasiliades, Michalis A. ^{[2
]}

Yan, Qinghua ^{[3
]}

Yang, Guangpeng ^{[4
]}

Du, Xuesen ^{[4
]}

Zhang, Cheng ^{[1
]}

Li, Yuran ^{[5
]}

Zhu, Tingyu ^{[5
]}

Wang, Qiang ^{[1
]}

Efstathiou, Angelos M. ^{[2
]}

机构：

[1] Beijing Forestry Univ, Coll Environm Sci & Engn, 35 Qinghua East Rd, Beijing 100083, Peoples R China

[2] Univ Cyprus, Heterogeneous Catalysis Lab, Chem Dept, 1 Univ Ave,Univ Campus, CY-2109 Nicosia, Cyprus

[3] Qingdao Agr Univ, Coll Resource & Environm, Qingdao 266109, Peoples R China

[4] Chongqing Univ, Sch Energy & Power Engn, Minist Educ, Key Lab Low Grade Energy Utilizat Technol & Syst, Chongqing 400044, Peoples R China

[5] Chinese Acad Sci, Res Ctr Proc Pollut Control, Natl Engn Lab Hydromet Cleaner Prod Technol, Inst Proc Engn, Beijing 100190, Peoples R China

来源：

APPLIED CATALYSIS B-ENVIRONMENTAL | 2020年 / 277卷

基金：

中国国家自然科学基金;

关键词：

LDHs; NH3-SCR; MnOx-based catalyst; Co-based NH3-SCR; Transient kinetics; SELECTIVE CATALYTIC-REDUCTION; LOW-TEMPERATURE NH3-SCR; INITIO MOLECULAR-DYNAMICS; LAYERED DOUBLE HYDROXIDE; OXIDE-BASED CATALYSTS; MIXED-OXIDE; NITRIC-OXIDE; SULFUR RESISTANCE; REACTION PATHWAYS; N-2; SELECTIVITY;

D O I：

10.1016/j.apcatb.2020.119186

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：

A Co0.5Mn1Fe0.25Al0.75Ox-LDO catalyst was developed which showed excellent performance for the low-temperature NH3-SCR. NOx conversions 100% were achieved in the whole 100-250 degrees C range, while after 10-h operation at 150 degrees C with 100 ppm SO2/5 vol% H2O in the feed, the NOx conversion was maintained at 80%. This catalyst provided a much better N-2-selectivity than the Mn1Fe0.25Al0.75Ox-LDO and Mn1Al1Ox-LDO, especially at 150-300 degrees C. It was found that Co0.5Mn1Fe0.25Al0.75Ox possessed higher surface acidity and reducibility, while XPS analyses indicated an electron transfer between Co3+/Co2+ and Mn4+/Mn3+ redox cycles, leading to a much lower N2O formation, supported by Density Functional Theory (DFT) calculations. Detailed analysis of gas responses obtained upon various step-gas switches was performed, which allowed to measure the surface concentration and reactivity of preadsorbed NOx-s and NHx-s leading to N-2 and N2O. Transient kinetic and DFT studies strongly suggested likely mechanisms of NH3-SCR and the critical role of Co for N-2-selectivity enhancement.

引用

页数：19

共 97 条

[1] Cux-Nb1.1-x (x=0.45, 0.35, 0.25, 0.15) bimetal oxides catalysts for the low temperature selective catalytic reduction of NO with NH3 [J].

Ali, Sher ;

Chen, Liqiang ;

Li, Zhibin ;

Zhang, Tianrui ;

Li, Rui ;

Bakhtiar, Syed ul Hasnain ;

Leng, Xuesong ;

Yuan, Fulong ;

Niu, Xiaoyu ;

Zhu, Yujun .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 236 :25-35

[2] Kinetic modeling of NH3-SCR over a supported Cu zeolite catalyst using axial species distribution measurements [J].

Auvray, Xavier ;

Partridge, William ;

Choi, Jae-Soon ;

Pihl, Josh ;

Coehlo, Filipa ;

Yezerets, Aleksey ;

Kamasamudram, Krishna ;

Currier, Neal ;

Olsson, Louise .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2015, 163 :393-403

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

BLOCHL, PE .

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

[4] 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

[5] A general strategy for the in situ decoration of porous Mn-Co bi-metal oxides on metal mesh/foam for high performance de-NOx monolith catalysts [J].

Cai, Sixiang ;

Liu, Jie ;

Zha, Kaiwen ;

Li, Hongrui ;

Shi, Liyi ;

Zhang, Dengsong .

NANOSCALE, 2017, 9 (17) :5648-5657

[6] 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

[7] Improvement of Activity and SO2 Tolerance of Sn-Modified MnOx-CeO2 Catalysts for NH3-SCR at Low Temperatures [J].

Chang, Huazhen ;

Chen, Xiaoyin ;

Li, Junhua ;

Ma, Lei ;

Wang, Chizhong ;

Liu, Caixia ;

Schwank, Johannes W. ;

Hao, Jiming .

ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (10) :5294-5301

[8] Composition-activity effects of Mn-Ce-O composites on phenol catalytic wet oxidation [J].

Chen, H ;

Sayari, A ;

Adnot, A ;

Larachi, F .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2001, 32 (03) :195-204

[9] A novel highly active and sulfur resistant catalyst from Mn-Fe-Al layered double hydroxide for low temperature NH3-SCR [J].

Chen, Sining ;

Yan, Qinghua ;

Zhang, Cheng ;

Wang, Qiang .

CATALYSIS TODAY, 2019, 327 :81-89

[10] 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

← 1 2 3 4 5 6 7 8 9 10 →