Site-Engineered MnGa@In-CHA OXZEO Catalysts for Synergistic Methane and Nitrogen Oxides Abatement

The rapid growth of natural-gas vehicles (NGVs) necessitates robust catalysts for the simultaneous abatement of methane (CH<sub>4</sub>), nitrogen oxides (NO<i>x</i>), and carbon monoxide (CO) under fluctuating exhaust compositions. We reported a site-engineered MnGa@In-CHA OXZEO catalyst in which indium was confined within an SSZ-13 framework, and Ga<sub>2</sub>O<sub>3</sub> and Mn<sub>2</sub>O<sub>3</sub> phases were uniformly dispersed on its exterior. Mn<sub>2</sub>O<sub>3</sub> markedly enhanced redox capacity, driving NO → NO<sub>2</sub> oxidation and lowering the activation energy for C-H bond cleavage in CH<sub>4</sub>, while Ga<sub>2</sub>O<sub>3</sub> tuned the Brønsted acidity and mediated electron transfer among In, Mn, and Ga centers. In situ DRIFTS studies identified CH<sub>4</sub> activation at InO<sup>+</sup> sites as the rate-determining step and revealed key intermediates (CH<sub>3</sub>NO<sub>2</sub>) that bridged the NO<i>x</i> reduction and CH<sub>4</sub>/CO oxidation pathways. The optimal Mn<sub>1</sub>Ga<sub>1</sub>@In-CHA achieved ≥90% NO<i>x</i> conversion at 390 °C, CH<sub>4</sub> conversion at 495 °C, and complete CO oxidation at 300 °C under both lean and rich conditions. It also maintained high activity after 24 h in a humid feed and exhibited stable performance across a wide range of O<sub>2</sub> concentrations. These combined features─high activity, selectivity, stability, and adaptability─underscore the promise of MnGa@In-CHA catalysts for NGVs exhaust abatement and offer an important design strategy for multifunctional emission-control materials.

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Journal
Environmental Science & Technology
Published
2025-09-04
DOI
https://doi.org/10.1021/acs.est.5c06606
Citations
1
Primary Topic
Catalytic Processes in Materials Science
Type
article
Field-Weighted Citation Impact
0.52

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article

Site-Engineered MnGa@In-CHA OXZEO Catalysts for Synergistic Methane and Nitrogen Oxides Abatement

Min Xiao, Yunbo Yu, Yingao Zhang, Yun Zhong et al.
1 citations
Environmental Science & Technology
Catalytic Processes in Materials Science
0.52
article

Site-Engineered MnGa@In-CHA OXZEO Catalysts for Synergistic Methane and Nitrogen Oxides Abatement

Min Xiao, Yunbo Yu, Yingao Zhang, Yun Zhong, Luna Ruan, Yanshuang Zhang, Yong De Yan, Chunlei Zhang, Guangyan Xu, Zidi Yan, Hong He, Qiqi Cai
article en
1 citations

Abstract

The rapid growth of natural-gas vehicles (NGVs) necessitates robust catalysts for the simultaneous abatement of methane (CH<sub>4</sub>), nitrogen oxides (NO<i>x</i>), and carbon monoxide (CO) under fluctuating exhaust compositions. We reported a site-engineered MnGa@In-CHA OXZEO catalyst in which indium was confined within an SSZ-13 framework, and Ga<sub>2</sub>O<sub>3</sub> and Mn<sub>2</sub>O<sub>3</sub> phases were uniformly dispersed on its exterior. Mn<sub>2</sub>O<sub>3</sub> markedly enhanced redox capacity, driving NO → NO<sub>2</sub> oxidation and lowering the activation energy for C-H bond cleavage in CH<sub>4</sub>, while Ga<sub>2</sub>O<sub>3</sub> tuned the Brønsted acidity and mediated electron transfer among In, Mn, and Ga centers. In situ DRIFTS studies identified CH<sub>4</sub> activation at InO<sup>+</sup> sites as the rate-determining step and revealed key intermediates (CH<sub>3</sub>NO<sub>2</sub>) that bridged the NO<i>x</i> reduction and CH<sub>4</sub>/CO oxidation pathways. The optimal Mn<sub>1</sub>Ga<sub>1</sub>@In-CHA achieved ≥90% NO<i>x</i> conversion at 390 °C, CH<sub>4</sub> conversion at 495 °C, and complete CO oxidation at 300 °C under both lean and rich conditions. It also maintained high activity after 24 h in a humid feed and exhibited stable performance across a wide range of O<sub>2</sub> concentrations. These combined features─high activity, selectivity, stability, and adaptability─underscore the promise of MnGa@In-CHA catalysts for NGVs exhaust abatement and offer an important design strategy for multifunctional emission-control materials.

Environmental Science & TechnologyVol. 59(36)
University of Science and Technology of China (CN), Chinese Academy of Sciences (CN), State Key Joint Laboratory of Environment Simulation and Pollution Control (CN), Research Center for Eco-Environmental Sciences (CN), Academy of Innovation Management (RU)
National Natural Science Foundation of China, Chinese Academy of Sciences, National Key Research and Development Program of China
Openalex Percentile: Top 33%
Catalytic Processes in Materials Science
0.52
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