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Title: Implications of methanol disproportionation on catalyst lifetime for methanol-to-olefins conversion by HSSZ-13

Authors:
; ; ;
Publication Date:
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1420007
Grant/Contract Number:
SC0014468
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 346; Journal Issue: C; Related Information: CHORUS Timestamp: 2018-02-09 08:25:35; Journal ID: ISSN 0021-9517
Publisher:
Elsevier
Country of Publication:
United States
Language:
English

Citation Formats

Hwang, Andrew, Kumar, Manjesh, Rimer, Jeffrey D., and Bhan, Aditya. Implications of methanol disproportionation on catalyst lifetime for methanol-to-olefins conversion by HSSZ-13. United States: N. p., 2017. Web. doi:10.1016/j.jcat.2016.12.003.
Hwang, Andrew, Kumar, Manjesh, Rimer, Jeffrey D., & Bhan, Aditya. Implications of methanol disproportionation on catalyst lifetime for methanol-to-olefins conversion by HSSZ-13. United States. doi:10.1016/j.jcat.2016.12.003.
Hwang, Andrew, Kumar, Manjesh, Rimer, Jeffrey D., and Bhan, Aditya. Wed . "Implications of methanol disproportionation on catalyst lifetime for methanol-to-olefins conversion by HSSZ-13". United States. doi:10.1016/j.jcat.2016.12.003.
@article{osti_1420007,
title = {Implications of methanol disproportionation on catalyst lifetime for methanol-to-olefins conversion by HSSZ-13},
author = {Hwang, Andrew and Kumar, Manjesh and Rimer, Jeffrey D. and Bhan, Aditya},
abstractNote = {},
doi = {10.1016/j.jcat.2016.12.003},
journal = {Journal of Catalysis},
number = C,
volume = 346,
place = {United States},
year = {Wed Feb 01 00:00:00 EST 2017},
month = {Wed Feb 01 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1016/j.jcat.2016.12.003

Citation Metrics:
Cited by: 10works
Citation information provided by
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  • Graphical abstract: In this research nanostructured CeAPSO-34 was synthesized to explore the effect of TEAOH and morpholine on its physiochemical properties and MTO performance. Prepared catalysts were characterized with XRD, FESEM, BET, FTIR and NH3-TPD techniques. The results indicated that the nature of the template determines the physiochemical properties of CeAPSO-34 due to different rate of crystal growth. The catalyst obtained by using morpholine showed longer life time as well as sustaining light olefins selectivity at higher values. Furthermore, a comprehensive thermodynamic analysis of overall reactions network was carried out to address the major channels of methanol to olefins conversion.more » - Highlights: • Introduction of Ce into SAPO-34 framework. • Comparison of CeAPSO-34 synthesized using morpholine and TEAOH. • The nature of the template determines the physiochemical properties of CeAPSO-34. • Morpholine enhances catalyst lifetime in MTO process. • Presenting a complete reaction network for MTO process. - Abstract: TEAOH and morpholine were employed in synthesis of nanostructured CeAPSO-34 molecular sieve and used in methanol to olefins conversion. Prepared samples were characterized by XRD, FESEM, EDX, BET, FTIR and NH{sub 3}-TPD techniques. XRD patterns reflected the higher crystallinity of the catalyst synthesized with morpholine. The FESEM results indicated that the nature of the template determines the morphology of nanostructured CeAPSO-34 due to different rate of crystal growth. There was a meaningful difference in the strength of both strong and weak acid sites for CeAPSO-34 catalysts synthesized with TEAOH and morpholine templates. The catalyst synthesized with morpholine showed higher desorption temperature of both weak and strong acid sites evidenced by NH{sub 3}-TPD characterization. The catalyst obtained using morpholine template had the longer lifetime and sustained desired light olefins at higher values. A comprehensive thermodynamic analysis of overall reactions network was carried out to address the major channels of methanol to olefins conversion.« less
  • The conversions of methanol, dimethyl ether, ethylene, propene, 1-butene, and 3,3-dimethyl-1-butene by reaction on various H-ZSM-5 catalysts at 370 to 380/sup 0/C demonstrate the importance of a carbenium ion mechanism in the formation of various aliphatic (C/sub 1/ to C/sub 6/) and aromatic (C/sub 6/ to C/sub 10/) hydrocarbons. C/sub 2/ to C/sub 4/ olefin reactions occur in a way very similar to the classical conjunct polymerization of olefins. The initial step in the formation of aromatics is a concerted cycloaddition of an olefin and a carbenium ion which is favored by the unique structural properties of the zeolite. Frommore » correlations between the Si/Al ratio and yields in aromatics and C/sub 4/ aliphatics, it is proposed that strong acid sites are responsible for the dehydrocyclization of C/sub 6+/ olefins into aromatics. Some evidence is also presented for alkylation reactions. Some of the unique properties of H-ZSM-5 are apparently due to the combination of strongly acidic and molecular sieving properties. 6 figures, 6 tables.« less
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  • Reactor types for commercial-scale methanol-to-olefins (MTO) processes in the ethene mode, using a small-pore molecular-sieve catalyst, have been evaluated both qualitatively and quantitatively. A kinetic model has been developed via an iterative process of model formulation, parameter estimation, and model validation. The final model consists of 12 reactions involving 6 component lumps plus coke. Important factors are the occurrence of consecutive reactions and the effect of coke on both the activity and selectivity. This kinetic model has been implemented in mathematical models of various reactors for the estimation of product selectivities and main reactor dimensions. These formed the basis formore » a comparison of different reactor types for a commercial-scale process. A circulating fast fluidized-bed reactor and a turbulent fluidized-bed reactor emerged as the most promising reactor systems for MTO in the ethene mode; ethene/propene ratios of 1--1.5 can be achieved with realistic reactor dimensions.« less
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