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The direct oxidation of methane to methanol by nitrous oxide over Fe-ZSM-5

Record Type:	Electronic resources : Monograph/item
Title/Author:	The direct oxidation of methane to methanol by nitrous oxide over Fe-ZSM-5
Author:	Wood, Benjamin Rue.
Description:	129 p.
Notes:	Co-Chairs: Alexis T. Bell; Jeffrey A. Reimer.
Notes:	Source: Dissertation Abstracts International, Volume: 65-02, Section: B, page: 0893.
Contained By:	Dissertation Abstracts International65-02B.
Subject:	Engineering, Chemical.
Online resource:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3121759
ISBN:	0496691104

The direct oxidation of methane to methanol by nitrous oxide over Fe-ZSM-5
Wood, Benjamin Rue.

The direct oxidation of methane to methanol by nitrous oxide over Fe-ZSM-5 [electronic resource] - 129 p.

Co-Chairs: Alexis T. Bell; Jeffrey A. Reimer.

Thesis (Ph.D.)--University of California, Berkeley, 2003.

Both classes of samples were characterized by X-ray absorption spectroscopy. These studies suggest that Fe in the post-synthetic exchanged samples is present as isolated cations associated with framework Al. The Fe-O coordination number is about 4 and the Fe-Al coordination number is about 1, regardless of Fe/Al ratio. Fe in unactivated hydrothermally synthesized Fe-ZSM-5 was found to reside in tetrahedral positions within the MFI framework. However, after thermal activation the Fe migrates to extra-framework sites. When Al is included in the structure, the resulting extra-framework Fe is associated with framework Al in an environment similar to that observed in exchanged Fe-ZSM-5.

ISBN: 0496691104Subjects--Topical Terms:

226989
Engineering, Chemical.

The direct oxidation of methane to methanol by nitrous oxide over Fe-ZSM-5
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245 1 4 $a The direct oxidation of methane to methanol by nitrous oxide over Fe-ZSM-5 $h [electronic resource]
300 $a 129 p.
500 $a Co-Chairs: Alexis T. Bell; Jeffrey A. Reimer.
500 $a Source: Dissertation Abstracts International, Volume: 65-02, Section: B, page: 0893.
502 $a Thesis (Ph.D.)--University of California, Berkeley, 2003.
520 # $a Both classes of samples were characterized by X-ray absorption spectroscopy. These studies suggest that Fe in the post-synthetic exchanged samples is present as isolated cations associated with framework Al. The Fe-O coordination number is about 4 and the Fe-Al coordination number is about 1, regardless of Fe/Al ratio. Fe in unactivated hydrothermally synthesized Fe-ZSM-5 was found to reside in tetrahedral positions within the MFI framework. However, after thermal activation the Fe migrates to extra-framework sites. When Al is included in the structure, the resulting extra-framework Fe is associated with framework Al in an environment similar to that observed in exchanged Fe-ZSM-5.
520 # $a IR spectroscopy was used to monitor the surface of Fe-ZSM-5 during the reaction of N2O and CH4. Surface methoxy groups were observed to replace hydroxyl groups on Fe and Si sites on Fe-ZSM-5. This work suggests that the active sites in the oxidation of CH4 to methoxy species by N2O consist of isolated extra-framework Fe species associated with framework Al. Surface methoxy groups were observed to decompose to CO upon heating in He or N2O. However, when H2O was introduced, surface methoxy species were hydrolyzed into the gas-phase as methanol.
520 # $a One possible route for the direct oxidation of CH4 to CH 3OH that has attracted attention is the oxidation of CH4 by N2O over Fe-ZSM-5 (an MFI structure with Al in tetrahedral framework positions and extra-framework Fe). The goal of the present work is to link structure to function in Fe-ZSM-5. For this work, Fe-ZSM-5 samples were made using the two synthetic methods, post-synthetic exchange and hydrothermal synthesis.
520 # $a Temperature-programmed and transient experiments were used to study the interaction of N2O with Fe-ZSM-5 and to determine several important kinetic parameters for N2O decomposition and surface oxygen loading. Nitrous Oxide was determined to adsorb on both Fe sites and Bronsted acid sites with heats of adsorption of 16 and 5 kcal/mol, respectively. For the stoichiometric decomposition of N2O to N2 and O 2, the apparent activation energy for both types of samples was &sim;44 kcal/mol. O2 desorption is calculated to be the most energetically demanding step in N2O decomposition.
590 $a School code: 0028.
650 # 0 $a Engineering, Chemical. $3 226989
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710 0 # $a University of California, Berkeley. $3 212474
773 0 # $g 65-02B. $t Dissertation Abstracts International
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790 1 0 $a Bell, Alexis T., $e advisor
790 1 0 $a Reimer, Jeffrey A., $e advisor
791 $a Ph.D.
792 $a 2003
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