Promoting effect of polyoxometallic acid modification on the NH3-SCR performance of Mn-based catalysts

被引:9
作者
Dong, Yi [1 ]
Ran, Mingchu [1 ]
Zhang, Xiao [1 ,2 ,3 ]
Lin, Saisai [1 ]
Li, Weixian [1 ]
Yang, Yang [1 ,3 ]
Song, Hao [1 ]
Wu, Weihong [1 ]
Liu, Shaojun [1 ]
Zheng, Chenghang [1 ,2 ,3 ]
Gao, Xiang [1 ,2 ,3 ]
机构
[1] Zhejiang Univ, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Peoples R China
[2] Baima Lake Lab, Hangzhou 310051, Peoples R China
[3] Zhejiang Univ, Jiaxing Res Inst, Jiaxing 314000, Peoples R China
来源
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING | 2024年 / 12卷 / 03期
基金
中国国家自然科学基金;
关键词
LT-SCR; Activity-selectivity trade-off; N2O formation inhibition; Transient reaction; NH3; oxidation; LOW-TEMPERATURE SCR; MNOX-CEO2; CATALYSTS; N-2; SELECTIVITY; SO2; TOLERANCE; N2O FORMATION; NO REDUCTION; NITRIC-OXIDE; NH3; MECHANISM; OXIDATION;
D O I
10.1016/j.jece.2024.112823
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The strong oxidation capabilities of Mn sites render Mn-based catalysts showing high activities of selective catalytic reduction (SCR) at temperatures < 250degree celsius, but simultaneously lead to the generation of by-product N2O with strong greenhouse effect. The activity-N-2-selectivity trade-off was a prevalent observation in the development of Mn-based SCR catalysts. Here, a polyoxometallic acid enhancement strategy was devised to simultaneously promote the N-2 selectivity and low-temperature SCR (LT-SCR) activity of Mn-based metal oxide catalysts, where the introduction of uniformly dispersed phosphomolybdic acid (HPMo) tuned the oxidation capabilities and enhanced NH3 adsorption-storage capability of catalysts. The combination of transient reaction, in-situ DRIFTS analysis and DFT calculations revealed that the main origin of N2O on the Mn-based catalysts was the deep oxidation of NH3, which was inhibited by the interaction between HPMo and Mn sites. Additional NH3 molecules adsorbed by the abundant acid sites supplied by HPMo further facilitated the SCR reaction. This strategy could guide the design of high-activity and high-selectivity LT-SCR catalysts for industrial denitration.
引用
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页数:10
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