Enhancing the Conversion Efficiency of Polyethylene to Methane through Codoping of Mn Atoms into Ru Centers and CeO<sub>2</sub> Supports
Chemical conversion has emerged as an effective approach for disposing waste plastics; however, the product diversity in traditional methods leads to pressing challenges in product separation and purification. As a pioneering advancement, the comprehensive transformation of waste plastics into CH<sub>4</sub> presents an attractive prospect: directly yielding high-purity products. Significantly, CH<sub>4</sub> is an important hydrogen carrier and an industrial feedstock. However, there is still much room for enhancing the overall efficiency. Herein, we show a new strategy to construct a high-efficiency and robust polyethylene (PE) upgrading catalyst by codoping Mn heteroatoms into both RuO<sub>2</sub> and CeO<sub>2</sub>. We found that these Mn heteroatoms effectively bolster the stability of Ru<sup>δ+</sup> species under high-temperature reduction conditions. The harmonious coexistence of Ru<sup>0</sup> and Ru<sup>δ+</sup> significantly refines the reaction pathway by enhancing the adsorption of the alkane intermediates. Consequently, we achieved an impressive PE conversion rate exceeding >99% with nearly 99% toward CH<sub>4</sub> at a moderate temperature of 250 °C within 8 h. Our discovery not only opens a new window for catalyst upgrading but also presents exciting opportunities for the in-depth conversion of waste plastics into complex, high-purity fine chemicals through methane-mediated catalysis.
Authors
- Shuyan Song (ORCID: https://orcid.org/0000-0002-7758-752X)
- Xiang‐Ping Chu (ORCID: https://orcid.org/0000-0002-6781-0468)
- Qing Xie (ORCID: https://orcid.org/0000-0001-8788-3237)
- Meng Zhao (ORCID: https://orcid.org/0000-0002-5163-1756)
- Yizhu Fang
- Lingling Zhang (ORCID: https://orcid.org/0000-0002-9390-8880)
- Xiao Wang (ORCID: https://orcid.org/0000-0002-5000-518X)
- Hongjie Zhang (ORCID: https://orcid.org/0000-0001-5433-8611)
- Fei Wang (ORCID: https://orcid.org/0000-0003-3475-1163)
- Lu Sun (ORCID: https://orcid.org/0000-0001-7041-1137)
Institutions
- University of Science and Technology of China (CN)
- Chinese Academy of Sciences (CN)
- Changchun Institute of Applied Chemistry (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-11-21
- DOI
- https://doi.org/10.1021/jacs.4c10793
- Citations
- 22
- Primary Topic
- Carbon dioxide utilization in catalysis
- Type
- article
- Field-Weighted Citation Impact
- 3.92
Funders
- National Natural Science Foundation of China
- People's Government of Jilin Province
- National Science and Technology Major Project
- Jilin Scientific and Technological Development Program