Mechanistic insight into the hydrogen transfer pathway for selective upcycling of PET to arenes
文献类型：期刊论文
| 作者 | Liu, Huiyu1,2,3,4; Zhang, Jun1,2,3,4; Gu, Jing1,2,3,4; Shan, Rui1,2,3,4; Yuan, Haoran1,2,3,4; Chen, Yong1,2,3,4 |
| 刊名 | JOURNAL OF CLEANER PRODUCTION
 |
| 出版日期 | 2023-11-01 |
| 卷号 | 425页码:10 |
| 关键词 | Polyethylene terephthalate Methanol Hydrogen transfer Hydrodeoxygenation Density functional theory calculation |
| ISSN号 | 0959-6526 |
| DOI | 10.1016/j.jclepro.2023.138924 |
| 通讯作者 | Yuan, Haoran(yuanhr@ms.giec.ac.cn) |
| 英文摘要 | Selective upcycling of waste plastics into value-added chemicals is of great significance for achieving the resource utilization. In the present study, the selective transformation of polyethylene terephthalate (PET) into arenes (benzene, toluene and p-xylene, labeled as BTX) via one-pot reaction in methanol without external hydrogen supply was put forward, which included methanol reforming, PET methanolysis and following in-situ hydrodeoxygenation. Mechanistic insight into the hydrogen transfer pathway in methanol-mediated PET upcy-cling into BTX over Pt/TiO2 was systematically elucidated. Remarkably, isotope labeling experiments revealed that hydrogen atoms from methanol could be transferred to the aromatic rings, owing to the formation of electron-deficient sites during conjugation. Density functional theory (DFT) calculations further confirmed that the cleavage of C-O bond in PET methanolysis derivatives took precedence over direct saturation of C--O bond, followed by in-situ hydrodeoxygenation transformation for the production of BTX. Using Pt/TiO2 as catalyst for H-transfer upcycling of PET in methanol, desirable BTX yield of 77.96% could be achieved after 3 h reaction. The present research will supply a novel perspective for the high-value utilization of waste oxygen-rich plastics via hydrogen transfer manner. |
| 资助项目 | National Natural Science Foundation of China[51976223] ; National Natural Science Foundation of China[51976222] ; National Natural Science Foundation of China[52276219] ; Guangdong Basic and Applied Basic Research Foundation[2021B1515020068] ; Project of Science and Technology of Guangzhou[202201010328] ; Yangfan Plan Innovation Team of Guangdong Province[2017YT05N093] ; Youth Innovation Promotion Association CAS[2023367] |
| WOS研究方向 | Science & Technology - Other Topics ; Engineering ; Environmental Sciences & Ecology |
| 语种 | 英语 |
| WOS记录号 | WOS:001096938500001 |
| 出版者 | ELSEVIER SCI LTD |
| 资助机构 | National Natural Science Foundation of China ; Guangdong Basic and Applied Basic Research Foundation ; Project of Science and Technology of Guangzhou ; Yangfan Plan Innovation Team of Guangdong Province ; Youth Innovation Promotion Association CAS |
| 源URL | [http://ir.giec.ac.cn/handle/344007/40220]  |
| 专题 | 中国科学院广州能源研究所 |
| 通讯作者 | Yuan, Haoran |
| 作者单位 | 1.Chinese Acad Sci, Key Lab Renewable Energy, Guangzhou 510640, Peoples R China 2.Univ Sci & Technol China, Sch Energy Sci & Engn, Hefei 230022, Peoples R China 3.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Peoples R China 4.Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Peoples R China |
| 推荐引用方式 GB/T 7714 | Liu, Huiyu,Zhang, Jun,Gu, Jing,et al. Mechanistic insight into the hydrogen transfer pathway for selective upcycling of PET to arenes[J]. JOURNAL OF CLEANER PRODUCTION,2023,425:10. |
| APA | Liu, Huiyu,Zhang, Jun,Gu, Jing,Shan, Rui,Yuan, Haoran,&Chen, Yong.(2023).Mechanistic insight into the hydrogen transfer pathway for selective upcycling of PET to arenes.JOURNAL OF CLEANER PRODUCTION,425,10. |
| MLA | Liu, Huiyu,et al."Mechanistic insight into the hydrogen transfer pathway for selective upcycling of PET to arenes".JOURNAL OF CLEANER PRODUCTION 425(2023):10. |
入库方式： OAI收割
来源：广州能源研究所
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