Promoting effects of desilication and dealumination on the catalytic performance of Al-rich HMOR for catalysing naphthalene tert-butylation with tertiary butanol
Zhang, Xiaomin1; Lu, Peng1; Xu, Lanjian1,2; Yuan, Yangyang1; Xu, Lei1; Huang, Zhihua1,2; Zhang, Jie1,2; Han, Qiao1,2,3,4
刊名APPLIED CATALYSIS A-GENERAL
2019-02-25
卷号572页码:80-89
关键词Naphthalene alkylation MOR zeolite Desilication Dealumination Coke deactivation
ISSN号0926-860X
DOI10.1016/j.apcata.2018.12.033
通讯作者Yuan, Yangyang(yuanyangyang@dicp.ac.cn) ; Xu, Lei(leixu@dicp.ac.cn)
英文摘要tert-Butylation of naphthalene is a potential technology to produce 2,6-di-tert-butylnaphthalene (2,6-DTBN), which is a valuable raw material for the synthesis of polyethylene naphthalate (PEN). Alkaline, acid and combined alkaline-acid treatments were adopted to regulate the porosity and acidity of Al-rich HMOR zeolite. The structure, porosity and acidity of the catalysts were well characterized and the catalytic performance in the tertbutylation of naphthalene was extensively investigated. The strong acid sites were verified as the intrinsic active sites for naphthalene alkylation for the first time. Characterization results indicated that alkaline treatment could extract silicon from the framework and intra-crystalline mesopores with diameters of 3-30 nm were successfully generated in Al-rich HMOR by one-step alkaline treatment. The introduced mesopores could enhance the mass diffusion of molecules as well as the coke-resistance, despite that the high acid density in the internal surface would lead to fast coke deposition. On the other hand, the acid treatment could remove the aluminium efficiently, leading to significantly decreased strong acid sites located at the micropores and pore entrances, which reduced coke deposition in the channels and pore entrances and brought about sharp increase in the conversion rate of naphthalene per strong acid site. Thus, higher naphthalene conversion and di-tert-butyl naphthalene (DTBN) selectivity were obtained over all the post-treated samples. Besides, the high selectivity for 2,6-DTBN (2,6-/2,7-DTBN > 28.0) remained. More importantly, combined alkaline and acid treatment had synergistic effects on the improvement of the initial activity as well as the catalytic stability due to the optimized acidity and porosity.
资助项目National Natural Science Foundation of China[21576252] ; National Natural Science Foundation of China[21506202]
WOS关键词LARGE-PORE ZEOLITES ; SHAPE-SELECTIVE ALKYLATION ; LIQUID-PHASE ALKYLATION ; H-MORDENITE ; MFI ZEOLITES ; REGIOSELECTIVE DIALKYLATION ; ACID PROPERTIES ; ALUMINUM ; ISOPROPYLATION ; ISOMERIZATION
WOS研究方向Chemistry ; Environmental Sciences & Ecology
语种英语
出版者ELSEVIER SCIENCE BV
WOS记录号WOS:000458471000010
资助机构National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
内容类型期刊论文
源URL[http://cas-ir.dicp.ac.cn/handle/321008/166034]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Yuan, Yangyang; Xu, Lei
作者单位1.Chinese Acad Sci, Dalian Inst Chem Phys, Natl Lab Clean Energy, Dalian 116023, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
3.Dalian Univ Technol, Dept Catalyt Chem & Engn, Dalian 116012, Peoples R China
4.Dalian Univ Technol, State Key Lab Fine Chem, Dalian 116012, Peoples R China
推荐引用方式
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Zhang, Xiaomin,Lu, Peng,Xu, Lanjian,et al. Promoting effects of desilication and dealumination on the catalytic performance of Al-rich HMOR for catalysing naphthalene tert-butylation with tertiary butanol[J]. APPLIED CATALYSIS A-GENERAL,2019,572:80-89.
APA Zhang, Xiaomin.,Lu, Peng.,Xu, Lanjian.,Yuan, Yangyang.,Xu, Lei.,...&Han, Qiao.(2019).Promoting effects of desilication and dealumination on the catalytic performance of Al-rich HMOR for catalysing naphthalene tert-butylation with tertiary butanol.APPLIED CATALYSIS A-GENERAL,572,80-89.
MLA Zhang, Xiaomin,et al."Promoting effects of desilication and dealumination on the catalytic performance of Al-rich HMOR for catalysing naphthalene tert-butylation with tertiary butanol".APPLIED CATALYSIS A-GENERAL 572(2019):80-89.
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