Chloromethane to olefins over H-SAPO-34: Probing the hydrocarbon pool mechanism

Fickel, Dustin W.; Sabnis, Kaiwalya D.; Li, Luanyi; Kulkarni, Neeta; Winter, Lea R.; Yan, Binhang; Chen, Jingguang G.

doi:10.1016/j.apcata.2016.09.004

Title: Chloromethane to olefins over H-SAPO-34: Probing the hydrocarbon pool mechanism

Journal Article · Fri Sep 09 00:00:00 EDT 2016 · Applied Catalysis. A, General

DOI:https://doi.org/10.1016/j.apcata.2016.09.004· OSTI ID:1341680

Fickel, Dustin W. ^[1]; Sabnis, Kaiwalya D. ^[1]; Li, Luanyi ^[1]; Kulkarni, Neeta ^[1]; Winter, Lea R. ^[2]; Yan, Binhang ^[3]; Chen, Jingguang G. ^[4]

SABIC Technology Center, Sugar Land, TX (United States)
Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.

In this paper, by means of in situ FTIR and ex situ¹³C NMR studies, the initial periods of the chloromethane-to-olefins (CTO) reaction over SAPO-34 were probed in order to investigate the activation period of the reaction and to elucidate the formation of the catalyst active site. A methylated benzene species has been observed to form during the initial activation period of the reaction, and a direct positive correlation was constructed between the formation of this species and the catalytic activity. The data thus indicate that these methylated benzene species contribute to the formation of active sites within SAPO-34 for the CTO reaction. This is the first known report identifying a direct semi-quantitative correlation between the catalyst activity and growth of a methylated benzene active species, during the activation period of the chloromethane to olefins reaction. Finally, the findings here in correspond well to those reported for the methanol to olefins reaction, suggesting that a similar ‘hydrocarbon pool’ mechanism may be responsible for the formation of light olefins in CTO chemistry as well.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); SABIC Technology Center, Sugar Land, TX (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Contributing Organization:: Columbia Univ., New York, NY (United States)

Grant/Contract Number:: SC0012704

OSTI ID:: 1341680

Report Number(s):: BNL-113408-2017-JA; R&D Project: CO035; KC0302010

Journal Information:: Applied Catalysis. A, General, Vol. 527; ISSN 0926-860X

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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Kinetic and Deactivation Differences Among Methanol, Dimethyl Ether and Chloromethane as Stock for Hydrocarbons Valecillos, José; Manzano, Hegoi; Aguayo, Andrés T. ChemCatChem, Vol. 11, Issue 22 https://doi.org/10.1002/cctc.201902050	journal	October 2019
Kinetic and Deactivation Differences Among Methanol, Dimethyl Ether and Chloromethane as Stock for Hydrocarbons Valecillos, José; Manzano, Hegoi; Aguayo, Andrés T. ChemCatChem, Vol. 11, Issue 22 https://doi.org/10.1002/cctc.201901204	journal	October 2019

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Title: Chloromethane to olefins over H-SAPO-34: Probing the hydrocarbon pool mechanism

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