Insight into the reasons for enhanced NH3-SCR activity and SO2 tolerance of Mn-Co layered oxides

被引：54

作者：

Feng, Xiangbo ^{[1
]}

Zhu, Jianru ^{[2
]}

Song, Kunli ^{[2
]}

Zeng, Jialing ^{[1
]}

Zhou, Xinya ^{[2
]}

Lin, Kexin ^{[2
]}

Guo, Xuanlin ^{[2
]}

Zhang, Cuihong ^{[1
]}

Xie, Chong ^{[3
]}

Shi, Jian-Wen ^{[2
]}

机构：

[1] Xijing Univ, Technol Inst Mat & Energy Sci TIMES, Sch Elect Informat, Xian Key Lab Adv Photoelect Mat & Energy Convers D, Xian 710123, Peoples R China

[2] Xi An Jiao Tong Univ, Ctr Nanomat Renewable Energy, Sch Elect Engn, State Key Lab Elect Insulat & Power Equipment, Xian 710049, Shaanxi, Peoples R China

[3] Xian Univ Technol, Inst Adv Electrochem Energy, Sch Mat Sci & Engn, Xian Key Lab New Energy Mat & Devices, Xian 710048, Shaanxi, Peoples R China

来源：

SEPARATION AND PURIFICATION TECHNOLOGY | 2024年 / 336卷

基金：

中国国家自然科学基金;

关键词：

Selective catalytic reduction; De-NOx activity; SO2; tolerance; Layered double hydroxides; Low temperature; SELECTIVE CATALYTIC-REDUCTION; LOW-TEMPERATURE NH3-SCR; MNOX-CEO2; CATALYSTS; FLUE-GAS; NOX; NH3; PERFORMANCE; MECHANISM; REMOVAL; NI;

D O I：

10.1016/j.seppur.2024.126285

中图分类号：

TQ [化学工业];

学科分类号：

0817 ;

摘要：

Mn-based catalysts have a fatal flaw in selective catalytic reduction (SCR) of NOx with NH3, which is poor SO2 tolerance. In this work, we successfully fabricated Mn-Co layered double oxides (LDOs) by calcining the Mn-Co layered double hydroxides (LDHs) generated by a hydrothermal method using urea solution. The obtained Mn-Co LDO presents excellent catalytic activity and SO2 tolerance in the SCR reaction of NOx with NH3. The enhanced activity can be attributed to the special surface physicochemical properties endowed by its LDO structure, such as large specific surface area, more exposed active sites, relatively high Mn4+ and O alpha/(O alpha + O beta) percentage, good reducibility, and abundant acidic sites. The enhanced SO2 tolerance can be ascribed to the weak adsorption energy of SO2 on Mn-Co LDO, which makes it difficult for SO2 to interact with the active sites. Furthermore, the NH3-SCR of NOx reaction that occurs on the surface of the MnCo-LDO follows both Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms. This study shines light on the design of Mn-based de-NOx catalysts with excellent SO2 tolerance.

引用

页数：10

共 67 条

[41] NiyCo1-yMn2Ox microspheres for the selective catalytic reduction of NOx with NH3: The synergetic effects between Ni and Co for improving low-temperature catalytic performance [J].

Shi, Jian-Wen ;

Gao, Ge ;

Fan, Zhaoyang ;

Gao, Chen ;

Wang, Baorui ;

Wang, Yao ;

Li, Zhihui ;

He, Chi ;

Niu, Chunming .

APPLIED CATALYSIS A-GENERAL, 2018, 560 :1-11

[42] Mechanism, performance and modification methods for NH3-SCR catalysts: A review [J].

Shi, Zhiwei ;

Peng, Qingguo ;

E, Jiaqiang ;

Xie, Bo ;

Wei, Jia ;

Yin, Ruixue ;

Fu, Guang .

FUEL, 2023, 331

[43] Low-temperature selective catalytic reduction of NOx with NH3: Exploring the mechanism of enhancing H2O tolerance through methylation functionalization and structural regulation in IPAx-Mn-BTC [J].

Song, Kunli ;

Hu, Jiyuan ;

Lu, Peng ;

Ma, Dandan ;

Zhou, Xinya ;

Li, Jun ;

Jiang, Ting ;

Li, Lu ;

Wu, Shangyuan ;

Shi, Jian-Wen .

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY, 2024, 343

[44] Insight into the Origin of Excellent SO2 Tolerance and de-NOx Performance of quasi-Mn-BTC in the Low-Temperature Catalytic Reduction of Nitrogen Oxide [J].

Song, Kunli ;

Guo, Kaiyu ;

Mao, Siman ;

Ma, Dandan ;

Lv, Yixuan ;

He, Chi ;

Wang, Hongkang ;

Cheng, Yonghong ;

Shi, Jian-Wen .

ACS CATALYSIS, 2023, 13 (07) :5020-5032

[45] Rational Regulation of Reducibility and Acid Site on Mn-Fe-BTC to Achieve High Low-Temperature Catalytic Denitration Performance [J].

Song, Kunli ;

Guo, Kaiyu ;

Lv, Yixuan ;

Ma, Dandan ;

Cheng, Yonghong ;

Shi, Jian-Wen .

ACS APPLIED MATERIALS & INTERFACES, 2023, 15 (03) :4132-4143

[46] Bimetallic modification of MnFeOx nanobelts with Nb and Nd for enhanced low-temperature de-NOx performance and SO2 tolerance [J].

Song, Kunli ;

Gao, Chen ;

Lu, Peng ;

Ma, Dandan ;

Cheng, Yonghong ;

Shi, Jian-Wen .

FUEL, 2023, 331

[47] Insights into the Sm/Zr co-doping effects on N2 selectivity and SO2 resistance of a MnOx-TiO2 catalyst for the NH3-SCR reaction [J].

Sun, Chuanzhi ;

Liu, Hao ;

Chen, Wei ;

Chen, Dezhan ;

Yu, Shuohan ;

Liu, Annai ;

Dong, Lin ;

Feng, Shuai .

CHEMICAL ENGINEERING JOURNAL, 2018, 347 :27-40

[48] Low temperature selective catalytic reduction of NOx with NH3 over amorphous MnOx catalysts prepared by three methods [J].

Tang, Xiaolong ;

Hao, Jiming ;

Xu, Wenguo ;

Li, Junhua .

CATALYSIS COMMUNICATIONS, 2007, 8 (03) :329-334

[49] Co-doping a metal (Cr, Fe, Co, Ni, Cu, Zn, Ce, and Zr) on Mn/TiO2 catalyst and its effect on the selective reduction of NO with NH3 at low-temperatures [J].

Thirupathi, Boningari ;

Smirniotis, Panagiotis G. .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2011, 110 :195-206

[50] One-pot synthesis of rare earth modified Cu/SAPO-34 for enhanced selective catalytic reduction denitration performance [J].

Wang, Baorui ;

Song, Kunli ;

Li, Zhenguo ;

Li, Kaixiang ;

Shi, Jian-Wen .

SEPARATION AND PURIFICATION TECHNOLOGY, 2022, 303

← 1 2 3 4 5 6 7 →