Unlocking High-Throughput Plasma-Catalytic Low-Temperature Oxidation of <i>n</i>-Hexane over Single-Atom Ag<sub>1</sub>/MnO<sub>2</sub> Catalysts
The total oxidation of <i>n</i>-hexane, a hazardous volatile organic compound (VOC) emitted by the pharmaceutical industry, presents a significant environmental challenge due to limited catalyst activity at low temperatures and poor stability at high temperatures. Here, we present a novel approach that overcomes these limitations by employing single-atom Ag<sub>1</sub>/MnO<sub>2</sub> catalysts coupled with nonthermal plasma (NTP). This strategy achieves exceptional performance in <i>n</i>-hexane oxidation at low temperatures, demonstrating 96.3% <i>n</i>-hexane removal and an energy yield of 74.1 g kW h<sup>-1</sup> with negligible byproduct formation (O<sub>3</sub> < 5 ppm, NO <sub><i>x</i></sub> < 20 ppm). In situ characterization of the plasma-catalytic system coupled with theoretical calculations revealed a synergistic mechanism for <i>n</i>-hexane oxidation. Reactive species generated by the NTP initiate the breakdown of <i>n</i>-hexane into smaller fragments. These fragments are then preferentially adsorbed onto the atomic Ag sites due to their favorable energetics, facilitating their subsequent oxidation. The incorporation of single Ag atoms not only enhances the selective adsorption of these NTP-generated intermediates but also accelerates the reaction kinetics. This work demonstrates the potential of single-atom catalysts coupled with NTP for efficient and environmentally friendly removal of VOCs at low temperatures. This approach offers a promising strategy for mitigating industrial air pollution and achieving cleaner air quality.
Authors
- Yaolin Wang (ORCID: https://orcid.org/0000-0003-1932-9810)
- Rino Morent (ORCID: https://orcid.org/0000-0001-6336-1485)
- Xin Cheng Tu (ORCID: https://orcid.org/0000-0002-6376-0897)
- Pengfei Xie (ORCID: https://orcid.org/0000-0002-7644-9934)
- Zhiping Ye (ORCID: https://orcid.org/0000-0003-0315-071X)
- Yan Mi (ORCID: https://orcid.org/0000-0002-2497-5342)
- Chuang Han (ORCID: https://orcid.org/0000-0002-2544-3655)
- Anton Yu Nikiforov (ORCID: https://orcid.org/0000-0002-2255-6419)
- Nathalie De Geyter (ORCID: https://orcid.org/0000-0001-7883-5786)
- Junhua Li (ORCID: https://orcid.org/0000-0001-7249-0529)
- Jun Chen (ORCID: https://orcid.org/0000-0003-2695-4673)
- Ke Wang (ORCID: https://orcid.org/0000-0002-1174-0907)
- Xuming Zhang (ORCID: https://orcid.org/0000-0003-4665-7641)
- Shulin Yang (ORCID: https://orcid.org/0000-0003-1511-2286)
- Jiade Wang (ORCID: https://orcid.org/0000-0002-9496-8551)
Institutions
- Zhejiang Sci-Tech University (CN)
- University of Liverpool (GB)
- Ghent University (BE)
- State Key Joint Laboratory of Environment Simulation and Pollution Control (CN)
- Zhejiang University of Technology (CN)
- Zhejiang University (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- JACS Au
- Published
- 2024-11-23
- DOI
- https://doi.org/10.1021/jacsau.4c00826
- Citations
- 3
- Primary Topic
- Catalytic Processes in Materials Science
- Type
- article
- Field-Weighted Citation Impact
- 0.35
Funders
- National Natural Science Foundation of China
- State Environmental Protection Key Laboratory of Sources and Control of Air Pollution Complex
- Engineering and Physical Sciences Research Council
- National Key Research and Development Program of China
- Natural Science Foundation of Zhejiang Province