Zhao Meng, Chu Xiang, Wang Fei, Fang Yizhu, Sun Lu, Xie Qing, Zhang Ling-Ling, Song Shuyan, Zhang Hongjie, Wang Xiao
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China.
School of Applied Chemistry and Engineering, University of Science and Technology of China, Hefei 230026, China.
J Am Chem Soc. 2024 Dec 4;146(48):33104-33111. doi: 10.1021/jacs.4c10793. Epub 2024 Nov 21.
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 presents an attractive prospect: directly yielding high-purity products. Significantly, CH 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 and CeO. We found that these Mn heteroatoms effectively bolster the stability of Ru species under high-temperature reduction conditions. The harmonious coexistence of Ru and Ru 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 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.
化学转化已成为处理废塑料的一种有效方法；然而，传统方法中的产物多样性给产物分离和提纯带来了紧迫的挑战。作为一项开创性进展，将废塑料全面转化为甲烷展现出诱人的前景：可直接得到高纯度产物。值得注意的是，甲烷是一种重要的氢载体和工业原料。然而，提高整体效率仍有很大空间。在此，我们展示了一种通过将锰杂原子共掺杂到氧化钌和氧化铈中来构建高效且稳定的聚乙烯升级催化剂的新策略。我们发现这些锰杂原子在高温还原条件下有效地增强了钌物种的稳定性。钌与钌的和谐共存通过增强烷烃中间体的吸附显著优化了反应路径。因此，在250℃的适中温度下8小时内，我们实现了令人印象深刻的聚乙烯转化率超过99%，生成甲烷的转化率接近99%。我们的发现不仅为催化剂升级打开了一扇新窗口，也为通过甲烷介导的催化将废塑料深度转化为复杂的高纯度精细化学品带来了令人兴奋的机遇。
