通过在Ru中心和CeO2载体上共掺杂Mn原子提高聚乙烯到甲烷的转化效率

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Meng Zhao, Xiang Chu, Fei Wang, Yizhu Fang, Lu Sun, Qing Xie, Ling-ling Zhang, Shuyan Song*, Hongjie Zhang and Xiao Wang*, 
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引用次数: 0

摘要

化学转化已成为处理废塑料的有效方法;然而,传统方法中产物的多样性给产物的分离和纯化带来了紧迫的挑战。废塑料综合转化CH4是一项开拓性的进步,具有诱人的前景: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。然而,整体效率仍有很大提升空间。在此,我们展示了一种新的策略,通过将Mn杂原子共掺杂到RuO2和CeO2中来构建高效坚固的聚乙烯(PE)升级催化剂。我们发现这些锰杂原子有效地增强了钌+在高温还原条件下的稳定性。Ru0和Ruδ+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,我们取得了令人印象深刻的PE转化率,超过99%,在250°C的中等温度下,在8小时内转化为CH4的转化率接近99%。我们的发现不仅为催化剂升级打开了新的窗口,而且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提供了令人兴奋的机会。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Enhancing the Conversion Efficiency of Polyethylene to Methane through Codoping of Mn Atoms into Ru Centers and CeO2 Supports

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 Ruδ+ species under high-temperature reduction conditions. The harmonious coexistence of Ru0 and Ruδ+ 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.

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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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