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

Abstract

In this paper, by means of in situ FTIR and ex situ 13C 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.

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [4]
  1. SABIC Technology Center, Sugar Land, TX (United States)
  2. Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
  4. Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering; Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Dept.
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); SABIC Technology Center, Sugar Land, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Contributing Org.:
Columbia Univ., New York, NY (United States)
OSTI Identifier:
1341680
Report Number(s):
BNL-113408-2017-JA
Journal ID: ISSN 0926-860X; R&D Project: CO035; KC0302010
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Applied Catalysis. A, General
Additional Journal Information:
Journal Volume: 527; Journal ID: ISSN 0926-860X
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; SAPO-34; Hydrocarbon pool; Chloromethane; Induction period; 13C NMR

Citation Formats

Fickel, Dustin W., Sabnis, Kaiwalya D., Li, Luanyi, Kulkarni, Neeta, Winter, Lea R., Yan, Binhang, and Chen, Jingguang G. Chloromethane to olefins over H-SAPO-34: Probing the hydrocarbon pool mechanism. United States: N. p., 2016. Web. doi:10.1016/j.apcata.2016.09.004.
Fickel, Dustin W., Sabnis, Kaiwalya D., Li, Luanyi, Kulkarni, Neeta, Winter, Lea R., Yan, Binhang, & Chen, Jingguang G. Chloromethane to olefins over H-SAPO-34: Probing the hydrocarbon pool mechanism. United States. doi:10.1016/j.apcata.2016.09.004.
Fickel, Dustin W., Sabnis, Kaiwalya D., Li, Luanyi, Kulkarni, Neeta, Winter, Lea R., Yan, Binhang, and Chen, Jingguang G. Fri . "Chloromethane to olefins over H-SAPO-34: Probing the hydrocarbon pool mechanism". United States. doi:10.1016/j.apcata.2016.09.004. https://www.osti.gov/servlets/purl/1341680.
@article{osti_1341680,
title = {Chloromethane to olefins over H-SAPO-34: Probing the hydrocarbon pool mechanism},
author = {Fickel, Dustin W. and Sabnis, Kaiwalya D. and Li, Luanyi and Kulkarni, Neeta and Winter, Lea R. and Yan, Binhang and Chen, Jingguang G.},
abstractNote = {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.},
doi = {10.1016/j.apcata.2016.09.004},
journal = {Applied Catalysis. A, General},
number = ,
volume = 527,
place = {United States},
year = {Fri Sep 09 00:00:00 EDT 2016},
month = {Fri Sep 09 00:00:00 EDT 2016}
}

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