Meng Zhao, Xiang Chu, Fei Wang, Yizhu Fang, Lu Sun, Qing Xie, Ling-ling Zhang, Shuyan Song, Hongjie Zhang, Xiao Wang
{"title":"通过在 Ru 中心和 CeO2 支持物中掺入锰原子提高聚乙烯到甲烷的转化效率","authors":"Meng Zhao, Xiang Chu, Fei Wang, Yizhu Fang, Lu Sun, Qing Xie, Ling-ling Zhang, Shuyan Song, Hongjie Zhang, Xiao Wang","doi":"10.1021/jacs.4c10793","DOIUrl":null,"url":null,"abstract":"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.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"1 1","pages":""},"PeriodicalIF":14.4000,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing the Conversion Efficiency of Polyethylene to Methane through Codoping of Mn Atoms into Ru Centers and CeO2 Supports\",\"authors\":\"Meng Zhao, Xiang Chu, Fei Wang, Yizhu Fang, Lu Sun, Qing Xie, Ling-ling Zhang, Shuyan Song, Hongjie Zhang, Xiao Wang\",\"doi\":\"10.1021/jacs.4c10793\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"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.\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"1 1\",\"pages\":\"\"},\"PeriodicalIF\":14.4000,\"publicationDate\":\"2024-11-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/jacs.4c10793\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.4c10793","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
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.
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.