WIPM OpenIR
Boosting the turnover number of core-shell Al-ZSM-5@B-ZSM-5 zeolite for methanol to propylene reaction by modulating its gradient acid site distribution and low consumption diffusion
Zhai, Yanliang1,2; Zhang, Shaolong1,2; Shang, Yunshan1,2; Song, Yu1,2; Wang, Wenxuan1,2; Ma, Tong1,2; Zhang, Luoming1,2; Gong, Yanjun1,2; Xu, Jun3; Deng, Feng3
2019-02-07
Source PublicationCATALYSIS SCIENCE & TECHNOLOGY
ISSN2044-4753
Volume9Issue:3Pages:659-671
AbstractHerein, a specific core-shell MFI zeolite was designed for the methanol to propylene (MTP) reaction. The core-shell structure of Al-ZSM-5@B-ZSM-5 and Al-ZSM-5@silicalite-1 were easily obtained via a two-step procedure, in which Al-ZSM-5 aggregate acted as the core and B-ZSM-5 or silicalite-1 as the shell. Their core-shell structures, acidity distribution and pore properties were characterized systemically, and new insights were gained into the synergetic effect of acid property and diffusion on the MTP reaction. The Al-ZSM-5@B-ZSM-5 zeolite exhibited a superior catalytic performance with a lifetime of 350 h (WHSV = 3 h(-1)), propylene selectivity of 49% and high turnover number of 4.3 x 10(6), while for the Al-ZSM-5 core, the corresponding values were 210 h, 43% and 5.2 x 10(5), respectively. Al-ZSM-5@silicalite-1 displayed the second best performance with the values of 250 h, 45% and 2.9 x 10(6), respectively. Gradient strong acid reduction from the core to the shell via the epitaxial growth of the silicalite-1 or B-ZSM-5 shell combined with an appropriate strong/weak acid ratio plays a vital role in inhibiting the hydrogen transfer reaction and thus gives a low consumption of propylene and low coke deposition. For the hydrogen transfer reaction of alkenes to form alkanes and aromatics, strong acid sites are required. Moreover, the acid sites originally existing on the external surface of the Al-ZSM-5 core were converted into internal acid sites due to the formation of an interface zone in the core-shell zeolite, possessing micropore characteristics, which in turn improve the shape selectivity and suppress coke deposition. Especially, the Al-ZSM-5@B-ZSM-5 zeolite displayed more weak acid sites and few strong acid sites on its shell surface, which are beneficial for the low formation of external coke and also account for the highest utilization of acid sites in the MTP reaction, high propylene selectivity and long lifetime.
Funding OrganizationState Key Development Program for Basic Research of China ; State Key Development Program for Basic Research of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; State Key Development Program for Basic Research of China ; State Key Development Program for Basic Research of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; State Key Development Program for Basic Research of China ; State Key Development Program for Basic Research of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; State Key Development Program for Basic Research of China ; State Key Development Program for Basic Research of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
DOI10.1039/c8cy02177e
WOS KeywordZSM-5 ZEOLITE ; HIERARCHICAL ZSM-5 ; COKE FORMATION ; CATALYTIC PERFORMANCE ; BORON INCORPORATION ; CRYSTALLITE SIZE ; HZSM-5 ZEOLITE ; CONVERSION ; HYDROCARBONS ; H-ZSM-5
Language英语
Funding ProjectState Key Development Program for Basic Research of China[2012CB215002] ; National Natural Science Foundation of China[21276278] ; National Natural Science Foundation of China[U1662116]
Funding OrganizationState Key Development Program for Basic Research of China ; State Key Development Program for Basic Research of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; State Key Development Program for Basic Research of China ; State Key Development Program for Basic Research of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; State Key Development Program for Basic Research of China ; State Key Development Program for Basic Research of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; State Key Development Program for Basic Research of China ; State Key Development Program for Basic Research of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China
WOS Research AreaChemistry
WOS SubjectChemistry, Physical
WOS IDWOS:000459731200010
PublisherROYAL SOC CHEMISTRY
Citation statistics
Cited Times:2[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.wipm.ac.cn/handle/112942/14288
Collection中国科学院武汉物理与数学研究所
Corresponding AuthorGong, Yanjun
Affiliation1.China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
2.China Univ Petr, Key Lab Catalysis CNPC, Beijing 102249, Peoples R China
3.Chinese Acad Sci, Wuhan Inst Phys & Math, Wuhan 430071, Hubei, Peoples R China
Recommended Citation
GB/T 7714
Zhai, Yanliang,Zhang, Shaolong,Shang, Yunshan,et al. Boosting the turnover number of core-shell Al-ZSM-5@B-ZSM-5 zeolite for methanol to propylene reaction by modulating its gradient acid site distribution and low consumption diffusion[J]. CATALYSIS SCIENCE & TECHNOLOGY,2019,9(3):659-671.
APA Zhai, Yanliang.,Zhang, Shaolong.,Shang, Yunshan.,Song, Yu.,Wang, Wenxuan.,...&Deng, Feng.(2019).Boosting the turnover number of core-shell Al-ZSM-5@B-ZSM-5 zeolite for methanol to propylene reaction by modulating its gradient acid site distribution and low consumption diffusion.CATALYSIS SCIENCE & TECHNOLOGY,9(3),659-671.
MLA Zhai, Yanliang,et al."Boosting the turnover number of core-shell Al-ZSM-5@B-ZSM-5 zeolite for methanol to propylene reaction by modulating its gradient acid site distribution and low consumption diffusion".CATALYSIS SCIENCE & TECHNOLOGY 9.3(2019):659-671.
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