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Research Article

Dual single-atom Ce-Ti/MnO2 catalyst enhances low-temperature NH3-SCR performance with high H2O and SO2 resistance

Jingjing Song1,2,§Shaomian Liu2,§Yongjun Ji3( )Wenqing Xu2( )Jian Yu2Bing Liu4( )Wenxing Chen5( )Jianling Zhang2Lihua Jia1( )Tingyu Zhu2Ziyi Zhong6,7Guangwen Xu8Fabing Su2,8( )
College of Chemistry and Chemical Engineering, Qiqihaer University, Qiqihaer 161006, China
Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
School of Light Industry, Beijing Technology and Business University, Beijing 100048, China
Department of Chemical Engineering, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, China
School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China
Department of Chemical Engineering, Guangdong Technion-Israel Institute of Technology (GTIIT), Shantou 515063, China
Technion-Israel Institute of Technology (IIT), Haifa 32000, Israel
Institute of Industrial Chemistry and Energy Technology, Shenyang University of Chemical Technology, Shenyang 110142, China

§ Jingjing Song and Shaomian Liu contributed equally to this work.

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Graphical Abstract

The dual single-atom Ce-Ti/MnO2 catalyst was synthesized via ball-milling and calcination. Compared with the pure MnO2, single-atom Ce/MnO2, and Ti/MnO2 catalysts, Ce-Ti/MnO2 showed better catalytic performance in selective catalytic reduction of NOx with NH3 (NH3-SCR) at 100−150 °C, e.g., higher NO conversion and enhanced H2O- and SO2-resistance. The Ce-Ti dual atoms act as sacrificial sites to weaken the adsorption and binding of SO2 and H2O on the neighboring active Mn sites but promote the NH3 adsorption. These results provide a new understanding of the NH3-SCR catalysis.

Abstract

Mn-based catalysts have exhibited promising performance in low-temperature selective catalytic reduction of NOx with NH3 (NH3-SCR). However, challenges such as H2O- or SO2-induced poisoning to these catalysts still remain. Herein, we report an efficient strategy to prepare the dual single-atom Ce-Ti/MnO2 catalyst via ball-milling and calcination processes to address these issues. Ce-Ti/MnO2 showed better catalytic performance with a higher NO conversion and enhanced H2O- and SO2-resistance at a low-temperature window (100−150 °C) than the MnO2, single-atom Ce/MnO2, and Ti/MnO2 catalysts. The in situ infrared Fourier transform spectroscopy analysis confirmed there is no competitive adsorption between NOx and H2O over the Ce-Ti/MnO2 catalyst. The calculation results showed that the synergistic interaction of the neighboring Ce-Ti dual atoms as sacrificial sites weakens the ability of the active Mn sites for binding SO2 and H2O but enhances their binding to NH3. The insight obtained in this work deepens the understanding of catalysis for NH3-SCR. The synthesis strategy developed in this work is easily scaled up to commercialization and applicable to preparing other MnO2-based single-atom catalysts.

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Nano Research
Pages 299-308
Cite this article:
Song J, Liu S, Ji Y, et al. Dual single-atom Ce-Ti/MnO2 catalyst enhances low-temperature NH3-SCR performance with high H2O and SO2 resistance. Nano Research, 2023, 16(1): 299-308. https://doi.org/10.1007/s12274-022-4790-8
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Received: 09 June 2022
Revised: 17 July 2022
Accepted: 18 July 2022
Published: 11 August 2022
© Tsinghua University Press 2022
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