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

TY - JOUR

T1 - Dual single-atom Ce-Ti/MnO2 catalyst enhances low-temperature NH3-SCR performance with high H2O and SO2 resistance

AU - Song, Jingjing

AU - Liu, Shaomian

AU - Ji, Yongjun

AU - Xu, Wenqing

AU - Yu, Jian

AU - Liu, Bing

AU - Chen, Wenxing

AU - Zhang, Jianling

AU - Jia, Lihua

AU - Zhu, Tingyu

AU - Zhong, Ziyi

AU - Xu, Guangwen

AU - Su, Fabing

PY - 2022/8/11

Y1 - 2022/8/11

N2 - 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.

AB - 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.

KW - dual single atom catalyst

KW - Ce-Ti/MnO2

KW - selective catalytic reduction of NOx with NH3 (NH3-SCR)

KW - low-temperature performance

KW - H2O- and SO2-resistance

U2 - 10.1007/s12274-022-4790-8

DO - 10.1007/s12274-022-4790-8

M3 - 文章

SN - 1998-0124

JO - Nano Research

JF - Nano Research

ER -