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Title: Interfacial Active Sites for CO2 Assisted Selective Cleavage of C–C/C–H Bonds in Ethane

Abstract

Selective upgrading of underutilized ethane in shale gas with greenhouse gas CO2 can produce syngas via dry reforming (C–C bond scission) or ethylene via oxidative dehydrogenation (C–H bond scission). However, it remains challenging to identify active sites responsible for the selective bond cleavage in ethane due to the complexity of supported catalysts. Herein, the ethane-CO2 reaction over CeO2-supported catalysts was investigated to unravel the functions of distinct interfacial sites by combining kinetic measurements with in situ characterizations and calculations: the Pd/CeOx interface is responsible for supplying reactive oxygen species, electron-deficient oxygen species on Pd surface boosts the non-selective bond scission to produce syngas, electron-enriched oxygen in the FeOx/Pd interface enhances the selective scission of C–H bond to yield ethylene, and the FeOx/CeO2 interaction mediates oxygen supply and confines metal ensembles. Finally, the current work identifies opportunities for using different interfacial structures in upgrading abundant shale gas and CO2.

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1829341
Alternate Identifier(s):
OSTI ID: 1671160; OSTI ID: 1725764
Report Number(s):
BNL-220653-2020-JAAM
Journal ID: ISSN 2451-9294; S2451929420303612; PII: S2451929420303612
Grant/Contract Number:  
SC0012704; SC0012653; AC02-06CH11357; AC02-05CH11231; ACI-1548562
Resource Type:
Published Article
Journal Name:
Chem
Additional Journal Information:
Journal Name: Chem Journal Volume: 6 Journal Issue: 10; Journal ID: ISSN 2451-9294
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
03 NATURAL GAS; shale gase; ethane; CO2; syngas; ethylene; reforming; dehydrogenation; C-H/C-C bond; interfacial sites; in situ and/or operando techniques

Citation Formats

Xie, Zhenhua, Tian, Dong, Xie, Meng, Yang, Shi-Ze, Xu, Yuanguo, Rui, Ning, Lee, Ji Hoon, Senanayake, Sanjaya D., Li, Kongzhai, Wang, Hua, Kattel, Shyam, and Chen, Jingguang G. Interfacial Active Sites for CO2 Assisted Selective Cleavage of C–C/C–H Bonds in Ethane. United States: N. p., 2020. Web. doi:10.1016/j.chempr.2020.07.011.
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Xie, Zhenhua, Tian, Dong, Xie, Meng, Yang, Shi-Ze, Xu, Yuanguo, Rui, Ning, Lee, Ji Hoon, Senanayake, Sanjaya D., Li, Kongzhai, Wang, Hua, Kattel, Shyam, & Chen, Jingguang G. Interfacial Active Sites for CO2 Assisted Selective Cleavage of C–C/C–H Bonds in Ethane. United States. https://doi.org/10.1016/j.chempr.2020.07.011
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Xie, Zhenhua, Tian, Dong, Xie, Meng, Yang, Shi-Ze, Xu, Yuanguo, Rui, Ning, Lee, Ji Hoon, Senanayake, Sanjaya D., Li, Kongzhai, Wang, Hua, Kattel, Shyam, and Chen, Jingguang G. Thu . "Interfacial Active Sites for CO2 Assisted Selective Cleavage of C–C/C–H Bonds in Ethane". United States. https://doi.org/10.1016/j.chempr.2020.07.011.
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@article{osti_1829341,
title = {Interfacial Active Sites for CO2 Assisted Selective Cleavage of C–C/C–H Bonds in Ethane},
author = {Xie, Zhenhua and Tian, Dong and Xie, Meng and Yang, Shi-Ze and Xu, Yuanguo and Rui, Ning and Lee, Ji Hoon and Senanayake, Sanjaya D. and Li, Kongzhai and Wang, Hua and Kattel, Shyam and Chen, Jingguang G.},
abstractNote = {Selective upgrading of underutilized ethane in shale gas with greenhouse gas CO2 can produce syngas via dry reforming (C–C bond scission) or ethylene via oxidative dehydrogenation (C–H bond scission). However, it remains challenging to identify active sites responsible for the selective bond cleavage in ethane due to the complexity of supported catalysts. Herein, the ethane-CO2 reaction over CeO2-supported catalysts was investigated to unravel the functions of distinct interfacial sites by combining kinetic measurements with in situ characterizations and calculations: the Pd/CeOx interface is responsible for supplying reactive oxygen species, electron-deficient oxygen species on Pd surface boosts the non-selective bond scission to produce syngas, electron-enriched oxygen in the FeOx/Pd interface enhances the selective scission of C–H bond to yield ethylene, and the FeOx/CeO2 interaction mediates oxygen supply and confines metal ensembles. Finally, the current work identifies opportunities for using different interfacial structures in upgrading abundant shale gas and CO2.},
doi = {10.1016/j.chempr.2020.07.011},
journal = {Chem},
number = 10,
volume = 6,
place = {United States},
year = {Thu Oct 01 00:00:00 EDT 2020},
month = {Thu Oct 01 00:00:00 EDT 2020}
}
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https://doi.org/10.1016/j.chempr.2020.07.011
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