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.
Authors
- Min Xiao (ORCID: https://orcid.org/0000-0002-8992-153X)
- Yunbo Yu (ORCID: https://orcid.org/0000-0003-2935-0955)
- Yingao Zhang (ORCID: https://orcid.org/0000-0001-8589-8638)
- Yun Zhong
- Luna Ruan
- Yanshuang Zhang
- Yong De Yan (ORCID: https://orcid.org/0009-0000-7523-466X)
- Chunlei Zhang (ORCID: https://orcid.org/0009-0005-3770-5914)
- Guangyan Xu (ORCID: https://orcid.org/0000-0002-4275-7517)
- Zidi Yan
- Hong He (ORCID: https://orcid.org/0000-0001-8476-8217)
- Qiqi Cai
Institutions
- 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)
Publication Details
- 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
Funders
- National Natural Science Foundation of China
- Chinese Academy of Sciences
- National Key Research and Development Program of China