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Title: Thermolytic Molecular Precursor Route to Site-IsolatedVanadia-Silica Materials and Their Catalytic Performance in MethaneSelective Oxidation

Abstract

The thermolytic molecular precursor (TMP) method was used to prepare site-isolated, high-surface area vanadia-silica (V/SBA15) materials of various V loadings via the grafting of two precursors, OV[OSi(O{sup t}Bu){sub 3}]{sub 3} (1) and Ov(O{sup t}Bu){sub 3} (2). Spectroscopic analysis indicates that excellent synthetic control was established for the exclusive formation of a pseudotetrahedral monovanadate (VO4) structure on all catalyst surfaces. Another V/SBA15 catalyst was prepared via conventional incipient wetness impregnation (WI) with aqueous NH4VO3. A spectroscopic investigation of this catalyst revealed the presence of monovanadate and polyvanadate species along with small domains of V2O5. The TMP materials behave as single-site catalysts in the selective oxidation of methane to formaldehyde up to a V coverage of 0.47 Vnm-2 and demonstrate superior activity compared with the WI catalyst. A space-time yield of 5.84 kgCH2Okg-1cat h-1 was observed, more than twice the highest value previously reported.

Authors:
; ; ;
Publication Date:
Research Org.:
Ernest Orlando Lawrence Berkeley NationalLaboratory, Berkeley, CA (US)
Sponsoring Org.:
USDOE Director. Office of Science. Basic EnergySciences
OSTI Identifier:
919832
Report Number(s):
LBNL-59613
Journal ID: ISSN 0021-9517; JCTLA5; R&D Project: 404201; BnR: KC0302010; TRN: US200822%%582
DOE Contract Number:
DE-AC02-05CH11231
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Catalysis; Journal Volume: 238; Related Information: Journal Publication Date: 2006
Country of Publication:
United States
Language:
English
Subject:
37; CATALYSTS; FORMALDEHYDE; IMPREGNATION; METHANE; OXIDATION; PERFORMANCE; PRECURSOR

Citation Formats

Ruddy, Daniel A., Ohler, Nicholas L., Bell, Alexis T., and Tilley, T.Don. Thermolytic Molecular Precursor Route to Site-IsolatedVanadia-Silica Materials and Their Catalytic Performance in MethaneSelective Oxidation. United States: N. p., 2005. Web.
Ruddy, Daniel A., Ohler, Nicholas L., Bell, Alexis T., & Tilley, T.Don. Thermolytic Molecular Precursor Route to Site-IsolatedVanadia-Silica Materials and Their Catalytic Performance in MethaneSelective Oxidation. United States.
Ruddy, Daniel A., Ohler, Nicholas L., Bell, Alexis T., and Tilley, T.Don. Wed . "Thermolytic Molecular Precursor Route to Site-IsolatedVanadia-Silica Materials and Their Catalytic Performance in MethaneSelective Oxidation". United States. doi:.
@article{osti_919832,
title = {Thermolytic Molecular Precursor Route to Site-IsolatedVanadia-Silica Materials and Their Catalytic Performance in MethaneSelective Oxidation},
author = {Ruddy, Daniel A. and Ohler, Nicholas L. and Bell, Alexis T. and Tilley, T.Don},
abstractNote = {The thermolytic molecular precursor (TMP) method was used to prepare site-isolated, high-surface area vanadia-silica (V/SBA15) materials of various V loadings via the grafting of two precursors, OV[OSi(O{sup t}Bu){sub 3}]{sub 3} (1) and Ov(O{sup t}Bu){sub 3} (2). Spectroscopic analysis indicates that excellent synthetic control was established for the exclusive formation of a pseudotetrahedral monovanadate (VO4) structure on all catalyst surfaces. Another V/SBA15 catalyst was prepared via conventional incipient wetness impregnation (WI) with aqueous NH4VO3. A spectroscopic investigation of this catalyst revealed the presence of monovanadate and polyvanadate species along with small domains of V2O5. The TMP materials behave as single-site catalysts in the selective oxidation of methane to formaldehyde up to a V coverage of 0.47 Vnm-2 and demonstrate superior activity compared with the WI catalyst. A space-time yield of 5.84 kgCH2Okg-1cat h-1 was observed, more than twice the highest value previously reported.},
doi = {},
journal = {Journal of Catalysis},
number = ,
volume = 238,
place = {United States},
year = {Wed Nov 23 00:00:00 EST 2005},
month = {Wed Nov 23 00:00:00 EST 2005}
}