Direct activation of CH4 to oxygenates and unsaturated hydrocarbons using N2O on Fe-modified zeolites

Kyung Soo Park, Jeong Hwa Kim, So Hyun Park, Dong Ju Moon, Hyunseog Roh, Chan Hwa Chung, Soong Ho Um, Joon Hwan Choi, Jong Wook Bae

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

Direct activation of CH4 to oxygenates and unsaturated light hydrocarbons was investigated using Fe-modified ZSM-5 and Ferrierite (FER) for a partial oxidation of CH4 with N2O oxidant. The amount of active α-oxygen sites and number of Bronsted acid sites on the Fe-modified zeolites were well correlated with CH4 conversion rate and product distributions. The amount of α-oxygen sites was largely changed according to preparation method such as wet impregnation or ion-exchange of iron precursor and types of zeolites. A large number of Bronsted acid sites and α-oxygen sites on the Fe-modified FER revealed a higher oxygenate formation such as methanol and dimethyl ether (DME) with COx, and a larger number of strong acid sites on Fe-modified ZSM-5 was also responsible for a higher selectivity to light hydrocarbons by a successive dehydration of oxygenates formed. The different catalytic performances were verified through proper measurements of the amount and type of acidic sites as well as the α-oxygen sites measured by N2O pulse chemisorption. The Fe-modified FER prepared by impregnation method possessed a larger amount of α-oxygen sites due to abundant Bronsted acid sites, which was responsible for a higher rate of CH4 conversion to oxygenates with the help of N2O decomposition on the α-oxygen sites originated from iron oxide nanoparticles.

Original languageEnglish
Pages (from-to)130-140
Number of pages11
JournalJournal of Molecular Catalysis A: Chemical
Volume426
DOIs
Publication statusPublished - 2017 Jan 1

Fingerprint

Zeolites
Hydrocarbons
zeolites
hydrocarbons
Chemical activation
activation
Oxygen
oxygen
Acids
acids
Impregnation
Chemisorption
Dehydration
Oxidants
Methanol
Reactive Oxygen Species
Ion exchange
Iron oxides
iron oxides
dehydration

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Process Chemistry and Technology
  • Physical and Theoretical Chemistry

Cite this

Park, Kyung Soo ; Kim, Jeong Hwa ; Park, So Hyun ; Moon, Dong Ju ; Roh, Hyunseog ; Chung, Chan Hwa ; Um, Soong Ho ; Choi, Joon Hwan ; Bae, Jong Wook. / Direct activation of CH4 to oxygenates and unsaturated hydrocarbons using N2O on Fe-modified zeolites. In: Journal of Molecular Catalysis A: Chemical. 2017 ; Vol. 426. pp. 130-140.
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Direct activation of CH4 to oxygenates and unsaturated hydrocarbons using N2O on Fe-modified zeolites. / Park, Kyung Soo; Kim, Jeong Hwa; Park, So Hyun; Moon, Dong Ju; Roh, Hyunseog; Chung, Chan Hwa; Um, Soong Ho; Choi, Joon Hwan; Bae, Jong Wook.

In: Journal of Molecular Catalysis A: Chemical, Vol. 426, 01.01.2017, p. 130-140.

Research output: Contribution to journalArticle

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T1 - Direct activation of CH4 to oxygenates and unsaturated hydrocarbons using N2O on Fe-modified zeolites

AU - Park, Kyung Soo

AU - Kim, Jeong Hwa

AU - Park, So Hyun

AU - Moon, Dong Ju

AU - Roh, Hyunseog

AU - Chung, Chan Hwa

AU - Um, Soong Ho

AU - Choi, Joon Hwan

AU - Bae, Jong Wook

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N2 - Direct activation of CH4 to oxygenates and unsaturated light hydrocarbons was investigated using Fe-modified ZSM-5 and Ferrierite (FER) for a partial oxidation of CH4 with N2O oxidant. The amount of active α-oxygen sites and number of Bronsted acid sites on the Fe-modified zeolites were well correlated with CH4 conversion rate and product distributions. The amount of α-oxygen sites was largely changed according to preparation method such as wet impregnation or ion-exchange of iron precursor and types of zeolites. A large number of Bronsted acid sites and α-oxygen sites on the Fe-modified FER revealed a higher oxygenate formation such as methanol and dimethyl ether (DME) with COx, and a larger number of strong acid sites on Fe-modified ZSM-5 was also responsible for a higher selectivity to light hydrocarbons by a successive dehydration of oxygenates formed. The different catalytic performances were verified through proper measurements of the amount and type of acidic sites as well as the α-oxygen sites measured by N2O pulse chemisorption. The Fe-modified FER prepared by impregnation method possessed a larger amount of α-oxygen sites due to abundant Bronsted acid sites, which was responsible for a higher rate of CH4 conversion to oxygenates with the help of N2O decomposition on the α-oxygen sites originated from iron oxide nanoparticles.

AB - Direct activation of CH4 to oxygenates and unsaturated light hydrocarbons was investigated using Fe-modified ZSM-5 and Ferrierite (FER) for a partial oxidation of CH4 with N2O oxidant. The amount of active α-oxygen sites and number of Bronsted acid sites on the Fe-modified zeolites were well correlated with CH4 conversion rate and product distributions. The amount of α-oxygen sites was largely changed according to preparation method such as wet impregnation or ion-exchange of iron precursor and types of zeolites. A large number of Bronsted acid sites and α-oxygen sites on the Fe-modified FER revealed a higher oxygenate formation such as methanol and dimethyl ether (DME) with COx, and a larger number of strong acid sites on Fe-modified ZSM-5 was also responsible for a higher selectivity to light hydrocarbons by a successive dehydration of oxygenates formed. The different catalytic performances were verified through proper measurements of the amount and type of acidic sites as well as the α-oxygen sites measured by N2O pulse chemisorption. The Fe-modified FER prepared by impregnation method possessed a larger amount of α-oxygen sites due to abundant Bronsted acid sites, which was responsible for a higher rate of CH4 conversion to oxygenates with the help of N2O decomposition on the α-oxygen sites originated from iron oxide nanoparticles.

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