Photonic Boosting of Lattice Oxygen Mobility in Rh–Mn/CoAlO<sub><b><i>x</i></b></sub> Heterostructure Catalysts to Enhanced CO-SCR Catalytic Performance

Developing efficient low-temperature selective catalytic reduction (CO-SCR) catalysts remains a key challenge in reducing nitrogen oxide (NO<sub><i>x</i></sub>) emissions. Here, we report a photothermal-enhanced Rh-Mn/CoAlO<sub><i>x</i></sub> heterostructure catalyst that achieves excellent NO conversion (more than 90% at 140 °C) and N<sub>2</sub> selectivity (>80%) under visible to infrared light irradiation. By integration of highly dispersed Rh units with Mn clusters onto a hydrotalcite-derived CoAlO<sub><i>x</i></sub> support, the catalyst exhibits synergistic light absorption and dynamic lattice oxygen migration capabilities. Through combined analysis using in situ DRIFTS, XAFS, XPS, EPR, and other techniques, we reveal that Mn doping induces numerous oxygen vacancies and promotes electron transfer between Rh and Mn, facilitating lattice oxygen activation via a mechanism similar to the Mars-van Krevelen mechanism. Light exposure reduces the activation energy and, according to Arrhenius analysis and NO-TPD results, accelerates the decomposition of nitrate intermediates and enhances the conversion rate of nitrous oxide to N<sub>2</sub>. Density functional theory (DFT) calculations confirm that N<sub>2</sub>O is more likely to be generated at the Rh-Mn interface, demonstrating its enhanced low-temperature activation ability for NO. This study innovatively enhances the catalytic performance of CO-SCR using light, providing a sustainable method for reducing low-energy NO<sub><i>x</i></sub> emissions.

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Journal
ACS Applied Materials & Interfaces
Published
2025-08-08
DOI
https://doi.org/10.1021/acsami.5c09789
Primary Topic
Catalytic Processes in Materials Science
Type
article
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0.00

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article

Photonic Boosting of Lattice Oxygen Mobility in Rh–Mn/CoAlOx Heterostructure Catalysts to Enhanced CO-SCR Catalytic Performance

Cheng Rao, Xinyu Han, Yibo Zhang, Qingwei Li et al.
ACS Applied Materials & Interfaces
Catalytic Processes in Materials Science
article

Photonic Boosting of Lattice Oxygen Mobility in Rh–Mn/CoAlOx Heterostructure Catalysts to Enhanced CO-SCR Catalytic Performance

Cheng Rao, Xinyu Han, Yibo Zhang, Qingwei Li, Xiangguang Yang, Kaiting Chen
article en

Abstract

Developing efficient low-temperature selective catalytic reduction (CO-SCR) catalysts remains a key challenge in reducing nitrogen oxide (NO<sub><i>x</i></sub>) emissions. Here, we report a photothermal-enhanced Rh-Mn/CoAlO<sub><i>x</i></sub> heterostructure catalyst that achieves excellent NO conversion (more than 90% at 140 °C) and N<sub>2</sub> selectivity (>80%) under visible to infrared light irradiation. By integration of highly dispersed Rh units with Mn clusters onto a hydrotalcite-derived CoAlO<sub><i>x</i></sub> support, the catalyst exhibits synergistic light absorption and dynamic lattice oxygen migration capabilities. Through combined analysis using in situ DRIFTS, XAFS, XPS, EPR, and other techniques, we reveal that Mn doping induces numerous oxygen vacancies and promotes electron transfer between Rh and Mn, facilitating lattice oxygen activation via a mechanism similar to the Mars-van Krevelen mechanism. Light exposure reduces the activation energy and, according to Arrhenius analysis and NO-TPD results, accelerates the decomposition of nitrate intermediates and enhances the conversion rate of nitrous oxide to N<sub>2</sub>. Density functional theory (DFT) calculations confirm that N<sub>2</sub>O is more likely to be generated at the Rh-Mn interface, demonstrating its enhanced low-temperature activation ability for NO. This study innovatively enhances the catalytic performance of CO-SCR using light, providing a sustainable method for reducing low-energy NO<sub><i>x</i></sub> emissions.

ACS Applied Materials & InterfacesVol. 17(33)
University of Science and Technology of China (CN), Jiangxi Academy of Environmental Sciences (CN)
National Natural Science Foundation of China, Chinese Academy of Sciences, People's Government of Jilin Province, Natural Science Foundation of Jiangxi Province, Youth Innovation Promotion Association of the Chinese Academy of Sciences, Key Research and Development Program of Jiangxi Province, National Key Research and Development Program of China
Responsible consumption and production
Openalex Percentile: Top 85%
Catalytic Processes in Materials Science
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