Citation: Xuebin Zhao, Yang Hong, Linying Wang, Dong Fan, Nana Yan, Xiaona Liu, Peng Tian, Xinwen Guo, Zhongmin Liu. External surface modification of as-made ZSM-5 and their catalytic performance in the methanol to propylene reaction[J]. Chinese Journal of Catalysis, ;2018, 39(8): 1418-1426. doi: 10.1016/S1872-2067(18)63117-1 shu

External surface modification of as-made ZSM-5 and their catalytic performance in the methanol to propylene reaction

Xuebin Zhao ^a,b,c, ,
Yang Hong ^b,c ,
Linying Wang ^b ,
Dong Fan ^b ,
Nana Yan ^b,c ,
Xiaona Liu ^b,c ,
Peng Tian ^b ,
Xinwen Guo ^a ,
Zhongmin Liu ^b

a State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning, China;
b National Engineering Laboratory for Methanol to Olefins, State Energy Low Carbon Catalysis and Engineering R & D Center, Dalian National Laboratory for Clean Energy, Collaborative Innovation Center of Chemistry for Energy Materials(iChEM), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
c University of Chinese Academy of Sciences, Beijing 100049, China

Received Date: 31 May 2018
Revised Date: 6 June 2018

Fund Project: This work was supported by the National Natural Science Foundation of China (21676262), and the Key Research Program of Frontier Sciences, CAS (QYZDB-SSW-JSC040).

Post-synthetic treatment of high-silica as-made ZSM-5 with organic template in the micropores was explored to reduce/remove the external surface acid density of ZSM-5. It is found that Na₂H₂EDTA treatment can selectively remove the surface Al atoms, but generates new acid sites (likely silanol nests) on the external surface. H₃PO₄ treatment is unable to remove surface Al atoms, while small amount of P is left on the external surface, which effectively decreases the acid density. The catalytic performance of the resultant materials is evaluated in the methanol conversion reaction. H₃PO₄ treatment can effectively improve both the catalytic lifetime and the stability of propene selectivity. This occurs due to a combination of the increased tolerance to the external coke deposition and the depressed coking rate (reduced side reactions). Na₂H₂EDTA treatment only prolongs the catalytic lifetime, resulting from the improved tolerance to the external coke deposition. Under the optimized H₃PO₄treatment condition, the resultant ZSM-5 gives a catalytic lifetime of about 1.5 times longer than the precursor. Moreover, the propene selectivity is improved, showing a slight increasing trend until the deactivation.
- Methanol to propene,
- ZSM-5 zeolite,
- Modification,
- Phosphoric acid,
- Ethylenediamine tetraacetic acid
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