Constructing the Al deficiency in Si-O(H)-Al units based on Pt/ZSM-5 for enhanced hydrocracking of polyethylene into high-quality liquid fuel | |
Zhong, Xia1,2; Liu, Jie1,3; Gao, Li1,2; Chen, Junnan1,2; Wang, Xiyang4; Zhang, Ying1,5; Wu, Yimin A.4; Shakeri, Mozaffar6; Zhang, Xia3; Zhang, Bingsen1,2 | |
通讯作者 | Zhang, Bingsen(bszhang@imr.ac.cn) |
2024-08-09 | |
发表期刊 | NANO RESEARCH
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ISSN | 1998-0124 |
页码 | 11 |
摘要 | Hydrocracking catalysis is a controllable route to plastic waste upgrading. However, the mismatched acid site-driven C-C cleavage and C=C hydrogenation process on metal restrict the efficiency and selectivity in conventional metal/acid bi-functional catalyst. Herein, we introduce Al deficiency in Si-O(H)-Al structural units of Pt/zeolite socony mobil-5 (Pt/ZSM-5) through discharge driven reduction (DR) process to precisely control the ratio of metal to acid, achieving hydrocracking of low-density polyethylene (LDPE) waste at 270 degrees C with 87.7% conversion and liquid fuel (C5-C21) selectivity of 77.8%. Pair distribution function (PDF) and nuclear magnetic resonance (NMR) spectroscopy demonstrate the partial absent Al sites further resulting short-range local disorder Si-O(H)-Al. Upon pyridine infrared spectroscopy (Py-IR) and CO diffuse reflectance Fourier-transform infrared (CO DRIFT) analysis, the extraction of Al modulates Br & oslash;nsted acid density of Pt/ZSM-5 with DR process (Pt/Z5DR), improves the interaction between Pt and ZSM-5 support, enhances the cationic of Pt. The metal-acid balance and electron-deficient Pt favor the matching speed of light olefins hydrogenation and the cracking of macromolecule intermediates. Moreover, density functional theory (DFT) calculations identify the thermodynamic stability of Pt/Z5DR and moderate adsorption capability towards light olefins. This work confirms the great potential of precisely controlled molar of metal to acid in metal/zeolite catalysts for LDPE upcycling, providing a viable path for dealing with PE plastic wastes. |
关键词 | plastic upcycling hydrocracking low-density polyethylene liquid fuel Pt zeolites |
资助者 | National Natural Science Foundation of China ; Iran National Science Foundation ; Research Fund of Shenyang National Laboratory for Materials Science |
DOI | 10.1007/s12274-024-6894-9 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | National Natural Science Foundation of China[52161145403] ; Iran National Science Foundation[4001399] ; Research Fund of Shenyang National Laboratory for Materials Science |
WOS研究方向 | Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics |
WOS类目 | Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied |
WOS记录号 | WOS:001287477300001 |
出版者 | TSINGHUA UNIV PRESS |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/188847 |
专题 | 中国科学院金属研究所 |
通讯作者 | Zhang, Bingsen |
作者单位 | 1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China 3.Northeastern Univ, Coll Sci, Dept Chem, Shenyang 110819, Peoples R China 4.Univ Waterloo, Waterloo Inst Nanotechnol, Dept Mech & Mechatron Engn, Waterloo, ON N2L 3G1, Canada 5.Liaoning Petrochem Univ, Sch Petrochem Engn, Fushun 113001, Peoples R China 6.Chem & Chem Engn Res Ctr Iran, Dept Chem & Petr Engn, Lab Heterogeneous Catalysis, Tehran 16363, Iran |
推荐引用方式 GB/T 7714 | Zhong, Xia,Liu, Jie,Gao, Li,et al. Constructing the Al deficiency in Si-O(H)-Al units based on Pt/ZSM-5 for enhanced hydrocracking of polyethylene into high-quality liquid fuel[J]. NANO RESEARCH,2024:11. |
APA | Zhong, Xia.,Liu, Jie.,Gao, Li.,Chen, Junnan.,Wang, Xiyang.,...&Zhang, Bingsen.(2024).Constructing the Al deficiency in Si-O(H)-Al units based on Pt/ZSM-5 for enhanced hydrocracking of polyethylene into high-quality liquid fuel.NANO RESEARCH,11. |
MLA | Zhong, Xia,et al."Constructing the Al deficiency in Si-O(H)-Al units based on Pt/ZSM-5 for enhanced hydrocracking of polyethylene into high-quality liquid fuel".NANO RESEARCH (2024):11. |
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