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Title: Dynamic modification of pore opening of SAPO-34 by adsorbed surface methoxy species during induction of catalytic methanol-to-olefins reactions

Abstract

Here, we report that the pore opening of SAPO-34 can be significantly modified by an adsorbed surface methoxy species during induction of the catalytic methanol-to-olefins process, which offers molecular sieving properties due to physical obstacle of the methoxy group and its adsorption modification to other hydrocarbons. X-ray powder diffraction and Rietveld refinement clearly reveal that the adsorbed single carbon atom as the methoxy group is dynamically created from methanol dehydration on a Brønsted acid site in close proximity to the pore windows. As a result, industrial desirable smaller olefins such as ethylene and propylene can be favourably made at the expenses of higher olefins. The structures and fundamental understanding in alteration in the olefins selectivity during induction may allow rational optimisation in catalytic performance under the complex fluidisation conditions.

Authors:
; ; ; ; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1457602
Report Number(s):
PNNL-SA-135309
Journal ID: ISSN 0926-3373; 49734; KC0302010
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Applied Catalysis. B, Environmental; Journal Volume: 237; Journal Issue: C
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Lo, B. T. W., Ye, L., Chang, G. G. Z., Purchase, K., Day, S., Tang, C. C., Mei, D., and Tsang, S. C. E.. Dynamic modification of pore opening of SAPO-34 by adsorbed surface methoxy species during induction of catalytic methanol-to-olefins reactions. United States: N. p., 2018. Web. doi:10.1016/j.apcatb.2018.05.090.
Lo, B. T. W., Ye, L., Chang, G. G. Z., Purchase, K., Day, S., Tang, C. C., Mei, D., & Tsang, S. C. E.. Dynamic modification of pore opening of SAPO-34 by adsorbed surface methoxy species during induction of catalytic methanol-to-olefins reactions. United States. doi:10.1016/j.apcatb.2018.05.090.
Lo, B. T. W., Ye, L., Chang, G. G. Z., Purchase, K., Day, S., Tang, C. C., Mei, D., and Tsang, S. C. E.. Sat . "Dynamic modification of pore opening of SAPO-34 by adsorbed surface methoxy species during induction of catalytic methanol-to-olefins reactions". United States. doi:10.1016/j.apcatb.2018.05.090.
@article{osti_1457602,
title = {Dynamic modification of pore opening of SAPO-34 by adsorbed surface methoxy species during induction of catalytic methanol-to-olefins reactions},
author = {Lo, B. T. W. and Ye, L. and Chang, G. G. Z. and Purchase, K. and Day, S. and Tang, C. C. and Mei, D. and Tsang, S. C. E.},
abstractNote = {Here, we report that the pore opening of SAPO-34 can be significantly modified by an adsorbed surface methoxy species during induction of the catalytic methanol-to-olefins process, which offers molecular sieving properties due to physical obstacle of the methoxy group and its adsorption modification to other hydrocarbons. X-ray powder diffraction and Rietveld refinement clearly reveal that the adsorbed single carbon atom as the methoxy group is dynamically created from methanol dehydration on a Brønsted acid site in close proximity to the pore windows. As a result, industrial desirable smaller olefins such as ethylene and propylene can be favourably made at the expenses of higher olefins. The structures and fundamental understanding in alteration in the olefins selectivity during induction may allow rational optimisation in catalytic performance under the complex fluidisation conditions.},
doi = {10.1016/j.apcatb.2018.05.090},
journal = {Applied Catalysis. B, Environmental},
number = C,
volume = 237,
place = {United States},
year = {Sat Dec 01 00:00:00 EST 2018},
month = {Sat Dec 01 00:00:00 EST 2018}
}