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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
ISSN1385-8947
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
DOI10.1016/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
被引频次:1[WOS]   [WOS记录]     [WOS相关记录]
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
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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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