Revisiting the NH3-SCR performance of MnO2 with different crystal phases: From electronic structure to catalytic activity
Manganese oxides are among the most promising low-temperature NH3-selective catalytic reduction (NH3-SCR) catalysts. MnO2 with different crystal phases (α-, β-, γ-, and δ-MnO2) exhibits significantly different NH3-SCR performance. The fundamental factors influencing the activity of MnO2 with differe...
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| Published in | Applied catalysis. B, Environmental Vol. 380; p. 125753 |
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| Main Authors | , , , , , , , , , |
| Format | Journal Article |
| Language | English |
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Elsevier B.V
01.01.2026
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| Abstract | Manganese oxides are among the most promising low-temperature NH3-selective catalytic reduction (NH3-SCR) catalysts. MnO2 with different crystal phases (α-, β-, γ-, and δ-MnO2) exhibits significantly different NH3-SCR performance. The fundamental factors influencing the activity of MnO2 with different crystal phases remain a subject of considerable debate. This study finds that β- and δ-MnO2 show poor activity due to low reactivity and poor NH3 adsorption. In contrast, α- and γ-MnO2 show high activity but differ in optimal reaction temperature windows. The smaller Mn-O coordination number and longer Mn-O bond distance in α-MnO2 result in an upward shift of its d-band center. Therefore, α-MnO2 exhibits stronger coupling between the Mn-d and N-p orbitals during NH3 adsorption, promoting *NH3 activation. As a result, α-MnO2 outperforms γ-MnO2 in low-temperature catalytic activity. This study reveals the impact of microscopic electronic orbital coupling on macroscopic catalytic performance, providing new insights for developing advanced low-temperature NH3-SCR catalysts.
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•Coordination environments cause SCR performance differences in MnO2 crystal phases.•d-Band shifts lead to varied NH3 activation barriers in α- and γ-MnO2.•Poor redox ability at low temperature makes β-MnO2 catalytically less active.•Nitrate buildup on δ-MnO2 inhibits SCR performance. |
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| AbstractList | Manganese oxides are among the most promising low-temperature NH3-selective catalytic reduction (NH3-SCR) catalysts. MnO2 with different crystal phases (α-, β-, γ-, and δ-MnO2) exhibits significantly different NH3-SCR performance. The fundamental factors influencing the activity of MnO2 with different crystal phases remain a subject of considerable debate. This study finds that β- and δ-MnO2 show poor activity due to low reactivity and poor NH3 adsorption. In contrast, α- and γ-MnO2 show high activity but differ in optimal reaction temperature windows. The smaller Mn-O coordination number and longer Mn-O bond distance in α-MnO2 result in an upward shift of its d-band center. Therefore, α-MnO2 exhibits stronger coupling between the Mn-d and N-p orbitals during NH3 adsorption, promoting *NH3 activation. As a result, α-MnO2 outperforms γ-MnO2 in low-temperature catalytic activity. This study reveals the impact of microscopic electronic orbital coupling on macroscopic catalytic performance, providing new insights for developing advanced low-temperature NH3-SCR catalysts.
[Display omitted]
•Coordination environments cause SCR performance differences in MnO2 crystal phases.•d-Band shifts lead to varied NH3 activation barriers in α- and γ-MnO2.•Poor redox ability at low temperature makes β-MnO2 catalytically less active.•Nitrate buildup on δ-MnO2 inhibits SCR performance. |
| ArticleNumber | 125753 |
| Author | Sun, Xiaoyu Wang, Houlin Xi, Yingwei Li, Junhua Yue, Yi Chen, Jianjun Gong, Zhengjun Xiong, Shangchao Ou, Hongjun Yang, Yi |
| Author_xml | – sequence: 1 givenname: Yi surname: Yue fullname: Yue, Yi organization: Sichuan Engineering Research Center for Pollution Control in Rail Transit Engineering, Sichuan International Science and Technology Cooperation base for Intelligent Environmental Protection and Sustainable Development in Rail Transit, School of Environmental Science and Engineering, Southwest Jiaotong University, Chengdu 610031, China – sequence: 2 givenname: Shangchao orcidid: 0000-0002-6523-0283 surname: Xiong fullname: Xiong, Shangchao email: xiongshangchao@swjtu.edu.cn organization: Sichuan Engineering Research Center for Pollution Control in Rail Transit Engineering, Sichuan International Science and Technology Cooperation base for Intelligent Environmental Protection and Sustainable Development in Rail Transit, School of Environmental Science and Engineering, Southwest Jiaotong University, Chengdu 610031, China – sequence: 3 givenname: Hongjun surname: Ou fullname: Ou, Hongjun organization: Sichuan Engineering Research Center for Pollution Control in Rail Transit Engineering, Sichuan International Science and Technology Cooperation base for Intelligent Environmental Protection and Sustainable Development in Rail Transit, School of Environmental Science and Engineering, Southwest Jiaotong University, Chengdu 610031, China – sequence: 4 givenname: Yi surname: Yang fullname: Yang, Yi organization: Sichuan Engineering Research Center for Pollution Control in Rail Transit Engineering, Sichuan International Science and Technology Cooperation base for Intelligent Environmental Protection and Sustainable Development in Rail Transit, School of Environmental Science and Engineering, Southwest Jiaotong University, Chengdu 610031, China – sequence: 5 givenname: Xiaoyu surname: Sun fullname: Sun, Xiaoyu organization: Sichuan Engineering Research Center for Pollution Control in Rail Transit Engineering, Sichuan International Science and Technology Cooperation base for Intelligent Environmental Protection and Sustainable Development in Rail Transit, School of Environmental Science and Engineering, Southwest Jiaotong University, Chengdu 610031, China – sequence: 6 givenname: Houlin surname: Wang fullname: Wang, Houlin organization: Sichuan Engineering Research Center for Pollution Control in Rail Transit Engineering, Sichuan International Science and Technology Cooperation base for Intelligent Environmental Protection and Sustainable Development in Rail Transit, School of Environmental Science and Engineering, Southwest Jiaotong University, Chengdu 610031, China – sequence: 7 givenname: Yingwei surname: Xi fullname: Xi, Yingwei organization: Sichuan Ecological Environment Monitoring Station, Chengdu 610091, China – sequence: 8 givenname: Zhengjun surname: Gong fullname: Gong, Zhengjun organization: Sichuan Engineering Research Center for Pollution Control in Rail Transit Engineering, Sichuan International Science and Technology Cooperation base for Intelligent Environmental Protection and Sustainable Development in Rail Transit, School of Environmental Science and Engineering, Southwest Jiaotong University, Chengdu 610031, China – sequence: 9 givenname: Jianjun surname: Chen fullname: Chen, Jianjun organization: State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China – sequence: 10 givenname: Junhua surname: Li fullname: Li, Junhua organization: State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China |
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| Keywords | MnO2 Reaction mechanism NH3-SCR Electronic structure NOx Low-temperature catalysts |
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