Melting-salt crystallization assisted controllable synthesis of core-shell zeolite catalyst for effective coupling of microwave hotspot and catalytic active site | |
Liu, Kai1; Ding, Qiuyan1; Wang, Na1; Kou, Zongliang1; Xu, Anran1; Li, Hong1; Zhao, Zhenyu1; Jiao, Yilai3; Gao, Xin1,2 | |
通讯作者 | Zhao, Zhenyu(zhaozhenyu2017@tju.edu.cn) ; Jiao, Yilai(yljiao@imr.ac.cn) ; Gao, Xin(gaoxin@tju.edu.cn) |
2024-04-01 | |
发表期刊 | CHEMICAL ENGINEERING JOURNAL
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ISSN | 1385-8947 |
卷号 | 485页码:14 |
摘要 | The applications of zeolites to microwave(MW)-assisted heterogeneous reactions are limited by their MWtransparent properties, which call for essential development of core-shell catalysts with MW-absorbing cores to utilize MW hotspots efficiently. However, current preparation methods fail to address the dilemmas of high heat transfer resistance and low heat generation efficiency caused by excessively thick zeolite shells and insufficient core filling. This study proposes an innovative ship-in-bottle strategy based on melting-salt crystallization for achieving controlled preparation of core-shell zeolite catalysts with ultra-thin shells and large filling rate of MW-absorbing cores. Based on the exploration of optimal conditions, ultra-thin hollow mesoporous zeolite shells around 30 nm thickness are successfully prepared, effectively reducing the heat transfer resistance from cores to catalytic sites. Subsequently, precise adjustment of the shell mesopore size enabled quantitative filling of MWabsorbing cores and therefore successful preparation of beta-MnO2@zeolite catalysts with significantly enhanced heat generation capabilities. Compared to conventional surface-loaded catalysts, the new core-shell catalysts improve toluene conversion by 44 % and paraxylene selectivity by 66 % in MW-assisted alkylation reactions. Fine numerical simulations of the catalyst heating process demonstrate that the excellent catalytic performance of core-shell catalysts is due to the effective coupling of MW hotspots and catalytic sites. |
关键词 | HZSM-5 zeolites Microwave heating Hotspot Structural design Core-shell catalysis |
资助者 | National Key R & D Programme of China ; National Nature Science Foundation of China ; Haihe Laboratory of Sustainable Chemical Transformations ; China Post-doctoral Science Foundation ; Tianjin University |
DOI | 10.1016/j.cej.2024.149985 |
收录类别 | SCI |
语种 | 英语 |
资助项目 | National Key R & D Programme of China[2023YFB3810600] ; National Nature Science Foundation of China[22222809] ; National Nature Science Foundation of China[22308250] ; Haihe Laboratory of Sustainable Chemical Transformations ; China Post-doctoral Science Foundation[2022TQ0232] ; China Post-doctoral Science Foundation[2022M722365] ; Tianjin University[2023XQM-0010] |
WOS研究方向 | Engineering |
WOS类目 | Engineering, Environmental ; Engineering, Chemical |
WOS记录号 | WOS:001202441200001 |
出版者 | ELSEVIER SCIENCE SA |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.imr.ac.cn/handle/321006/185511 |
专题 | 中国科学院金属研究所 |
通讯作者 | Zhao, Zhenyu; Jiao, Yilai; Gao, Xin |
作者单位 | 1.Tianjin Univ, Natl Engn Res Ctr Distillat Technol, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Sch Chem Engn & Technol, Tianjin 300350, Peoples R China 2.Haihe Lab Sustainable Chem Transformat, Tianjin 300192, Peoples R China 3.Chinese Acad Sci, Inst Met Res, 72 Wenhua Rd, Shenyang 110016, Peoples R China |
推荐引用方式 GB/T 7714 | Liu, Kai,Ding, Qiuyan,Wang, Na,et al. Melting-salt crystallization assisted controllable synthesis of core-shell zeolite catalyst for effective coupling of microwave hotspot and catalytic active site[J]. CHEMICAL ENGINEERING JOURNAL,2024,485:14. |
APA | Liu, Kai.,Ding, Qiuyan.,Wang, Na.,Kou, Zongliang.,Xu, Anran.,...&Gao, Xin.(2024).Melting-salt crystallization assisted controllable synthesis of core-shell zeolite catalyst for effective coupling of microwave hotspot and catalytic active site.CHEMICAL ENGINEERING JOURNAL,485,14. |
MLA | Liu, Kai,et al."Melting-salt crystallization assisted controllable synthesis of core-shell zeolite catalyst for effective coupling of microwave hotspot and catalytic active site".CHEMICAL ENGINEERING JOURNAL 485(2024):14. |
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