A stable spherical MOF-derived Mnx-Fe2O3/C catalysts for low-temperature CO-SCR

被引：16

作者：

Li, Cheng ^{[1
]}

Shi, Yong ^{[1
]}

Zhao, Qi Dong ^{[2
]}

Xiong, Wei ^{[1
]}

Ding, Yue ^{[1
]}

Sun, Jian Heng ^{[1
]}

Huang, Ying Lei ^{[1
]}

Zhao, Zhong Fei ^{[1
]}

机构：

[1] Dalian Univ Technol, Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn, Minist Educ, Dalian 116024, Peoples R China

[2] Dalian Univ Technol, Sch Chem Engn, Panjin Campus,2 Dagong Rd, Panjin, Peoples R China

来源：

CHEMICAL ENGINEERING JOURNAL | 2023年 / 475卷

基金：

中央高校基本科研业务费专项资金资助; 中国国家自然科学基金;

关键词：

CO-SCR; MOF-derived bimetallic oxides; Fe-O-Mn sites; METAL-ORGANIC FRAMEWORKS; EFFICIENT CATALYST; NO REDUCTION; PERFORMANCE; NH3-SCR; MN; OPTIMIZATION; MECHANISM; DESIGN; OXIDES;

D O I：

10.1016/j.cej.2023.146388

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

A series of spherical Mnx-Fe2O3/C catalysts derived from MnFe-MOF-74 were fabricated via a sacrificing tem -plate method and applied for CO-SCR. Among the tested catalysts, Mn0.5-Fe2O3/C catalysts achieved a maximum NO conversion of 100 % in a broad temperature range between 225 and 500 degrees C, significantly higher than monometallic Fe2O3/C. Based on TPR, BET and oS results, a redox reaction Fe3+ + Mn2+ <-> Fe2+ + Mn3+ over Fe-O-Mn sites was constructed, which greatly facilitated the adsorption and activation of NO molecules. DFT calculations revealed that the incorporation of Mn obviously increased the local electron density of Fe-Mn sites not only resulting in a strong C-Fe/Mn and N-Fe/Mn bonding, but also effectively weaken the N-O bond. And the NO adsorption energy of Fe-O-Mn site over Mn doped alpha-Fe2O3 is-0.87 eV which indicates the stability of the adsorption configuration. Combined with the in situ FT-IR results, important intermediates Fe2+-(NO)22- and N2O were identified respectively at 1261 and 1358 cm-1, which were promoted by the synergistic interaction of Mn and Fe. This Mn-Fe synergistic interaction could contribute to lowering reaction barrier and boosting CO-SCR performance.

引用

页数：12

共 62 条

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