Identifying the descriptor governing NO oxidation on mullite Sm(Y, Tb, Gd, Lu)Mn2O5 for diesel exhaust cleaning

被引：54

作者：

Li, Hao-Bo ^{[1
]}

Wang, Wei-Hua ^{[1
]}

Qian, Xinyu ^{[1
]}

Cheng, Yahui ^{[1
]}

Xie, Xinjian ^{[2
]}

Liu, Jieyu ^{[1
]}

Sun, Shuhui ^{[3
]}

Zhou, Jigang ^{[4
]}

Hu, Yongfeng ^{[4
]}

Xu, Jianping ^{[5
]}

Li, Lan ^{[5
]}

Zhang, Yan ^{[6
]}

Du, Xiwen ^{[6
]}

Gao, Kuanghong ^{[7
]}

Li, Zhiqing ^{[7
]}

Zhang, Cui ^{[8
]}

Wang, Shudong ^{[9
]}

Chen, Haijun ^{[9
]}

Zhao, Yidong ^{[10
]}

Lu, Feng ^{[1
]}

Wang, Weichao ^{[1
]}

Liu, Hui ^{[1
]}

机构：

[1] Nankai Univ, Dept Elect, Tianjin 300071, Peoples R China

[2] Univ Technol Tianjin, Sch Mat Sci & Engn Hebei, Tianjin 300401, Peoples R China

[3] Inst Natl Rech Sci, Varennes, PQ J3X 1S2, Canada

[4] Canadian Light Source, Saskatoon, SK S7N 2V3, Canada

[5] Tianjin Univ Technol, Coll Sci, Tianjin 300384, Peoples R China

[6] Tianjin Univ, Sch Mat Sci & Engn, Tianjin 300072, Peoples R China

[7] Tianjin Univ, Dept Phys, Tianjin 300072, Peoples R China

[8] Nankai Univ, Coll Chem, Tianjin 300071, Peoples R China

[9] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China

[10] Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China

来源：

CATALYSIS SCIENCE & TECHNOLOGY | 2016年 / 6卷 / 11期

基金：

中国国家自然科学基金;

关键词：

SELECTIVE CATALYTIC-REDUCTION; RAY-ABSORPTION SPECTROSCOPY; DENSITY-FUNCTIONAL THEORY; PEROVSKITES; OXIDES;

D O I：

10.1039/c5cy01798j

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：

The current fast selective catalytic reduction (fast-SCR) technology shows effectiveness in converting diesel engine generated nitrogen oxides (NOx) to environmentally benign nitrogen (N-2) with the aid of the precious metal catalyst platinum. Driven by the previous finding of the low-cost mullite's great superiority over Pt in terms of NO oxidation, a series of Mn-based oxides Sm(Y, Tb, Gd, Lu)Mn2O5 are synthesized to identify a general descriptor that governs the catalytic performance. Utilizing soft X-ray absorption characterization and molecular orbital theory, here, we show that the catalytic activity difference presents little dependence on the 3d electron occupancy when the A site element is varied (Sm, Tb, Y, Gd, Lu). Instead, strong p-d hybridization between lattice O and octahedral Mn leads to weak bonding strength between external O* and pyramid Mn and essentially increases the catalytic activity for converting NO to NO2.

引用

页码：3971 / 3975

页数：5

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