<br>通过将 Mn 原子共掺杂成 Ru 中心和 CeO2 载体来提高聚乙烯向甲烷的转化效率,Journal of the American Chemical Society

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通过将 Mn 原子共掺杂成 Ru 中心和 CeO2 载体来提高聚乙烯向甲烷的转化效率
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-11-21 , DOI: 10.1021/jacs.4c10793
Meng Zhao _{1,

2} , Xiang Chu _{1,

2} , Fei Wang ₁ , Yizhu Fang _{1,

2} , Lu Sun _{1,

2} , Qing Xie _{1,

2} , Ling-Ling Zhang _{1,

2} , Shuyan Song _{1,

2} , Hongjie Zhang _{1,

2,

3} , Xiao Wang _{1,

2}

Affiliation

化学转化已成为处理废塑料的有效方法;然而，传统方法中的产品多样性导致了产品分离和纯化方面的紧迫挑战。作为一项开创性的进步，将废塑料全面转化为 CH₄ 具有极具吸引力的前景：直接生产高纯度产品。值得注意的是，CH₄ 是一种重要的氢载体和工业原料。但是，整体效率的提升空间还很大。在此，我们展示了一种通过将 Mn 杂原子共掺杂成 RuO₂ 和 CeO₂ 来构建高效且强大的聚乙烯（PE）活化催化剂的新策略。我们发现这些 Mn 杂原子有效地增强了 Ru^δ+ 物质在高温还原条件下的稳定性。Ru⁰ 和 Ru^δ+ 的和谐共存通过增强烷烃中间体的吸附显著改善了反应途径。因此，在 250 °C 的中等温度下，我们在 8 小时内实现了超过 >99% 的 PE 转化率，其中近 99% 向 CH₄ 转换。我们的发现不仅为催化剂升级打开了一扇新窗口，而且还为通过甲烷介导的催化将废塑料深度转化为复杂、高纯度的精细化学品提供了令人兴奋的机会。

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Enhancing the Conversion Efficiency of Polyethylene to Methane through Codoping of Mn Atoms into Ru Centers and CeO2 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 CH₄ presents an attractive prospect: directly yielding high-purity products. Significantly, CH₄ 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 RuO₂ and CeO₂. We found that these Mn heteroatoms effectively bolster the stability of Ru^δ+ species under high-temperature reduction conditions. The harmonious coexistence of Ru⁰ and Ru^δ+ 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 CH₄ 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.

更新日期：2024-11-21

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