Probing the role of nanoconfinement in improving N2 selectivity of Mn-based catalysts during NH3-SCR

被引:1
|
作者
Zhu, Na [1 ]
Xu, Lichang [1 ]
Wang, Shuai [1 ]
Lian, Zhihua [2 ]
Shan, Wenpo [2 ,3 ]
机构
[1] Fuzhou Univ, Sch Adv Mfg, Fuzhou 362251, Jinjiang, Peoples R China
[2] Chinese Acad Sci, Inst Urban Environm, Key Lab Urban Pollutant Convers, Xiamen 361021, Peoples R China
[3] Chinese Acad Sci, Inst Urban Environm, Zhejiang Key Lab Urban Environm Proc & Pollut Cont, Ningbo Urban Environm Observat & Res Stn, Ningbo 315800, Peoples R China
基金
中国国家自然科学基金;
关键词
Selective catalytic reduction; Mn-based catalysts; TiO2; nanotubes; N-2; selectivity; INITIO MOLECULAR-DYNAMICS; OXIDE; REDUCTION; NOX; ENHANCEMENT; NANOTUBES; NH3; FE; CU;
D O I
10.1016/j.apsusc.2024.161282
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
Mn-based catalysts are promising low-temperature NH3-SCR catalysts, yet their strong oxidative capability leads to excessive N2O production, contributing to global warming. This study explored titanium nanotubes supported MnOx catalysts for NH3-SCR. The optimal catalyst, 10%Mn/TN showed remarkable NOx conversion over 95 % at 150-400 degrees C, together with a N-2 selectivity surpassing 95 % below 300 degrees C. In contrast, 10%Mn/Ti catalyst used for comparison had a N-2 selectivity as low as 30 %. The active Mn species may predominantly locate within the inner regions of the titanium nanotubes, which effectively regulated the redox properties of 10%Mn/TN. Density Functional Theory (DFT) calculations showed that the decomposition of NH4NO3 formed on 10%Mn/TN into H2O and N2O was more difficult than that on 10%Mn/Ti. Furthermore, the NH3-SCR reaction on 10%Mn/TN mainly followed the Eley-Rideal mechanism and NH4NO3 decomposition was effectively inhibited, consequently leading to a significant improvement in N-2 selectivity. These findings offer crucial insights for the design and development of Mn-based catalysts with superior activity and N-2 selectivity in NH3-SCR applications.
引用
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页数:10
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