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Title: Time-Resolved FT-IR Spectroscopy of CO Hydrogenation overSupported Ru Catalyst at 700K

Abstract

Time-resolved FT-IR spectra of carbon monoxide hydrogenation over alumina-supported ruthenium were recorded on the millisecond timescale at 703 K using various H{sub 2} concentrations (1 atm total pressure). Adsorbed carbon monoxide was detected along with gas phase products methane (3016 and 1306 cm{sup -1}), water (sharp bands from 1900 - 1300 cm{sup -1}), and carbon dioxide (2348 cm{sup -1}). No other surface species were detected other than adsorbed carbon monoxide. The rate of formation of methane (2.5 {+-} 0.4 s{sup -1}) coincides with the rate of formation of carbon dioxide (3.4 {+-} 0.6 s{sup -1}), and bands due to water are observed to grow in over time. These results establish that methane and carbon dioxide originate from the same intermediate. The adsorbed carbon monoxide band is broad and unsymmetrical with a maximum at 2010 cm{sup -1} in spectra observed at 36 ms that shifts over 3000 ms to 1960 cm{sup -1} due to decreasing amounts of adsorbed carbon monoxide. Kinetic analysis of the adsorbed carbon monoxide band reveals that only a portion of the band can be temporally linked to gas phase products that we observe over the first 1000 ms of catalysis. This result suggests that we are observingmore » dispersive kinetics, which is most likely due to heterogeneity of the surface environment.« less

Authors:
;
Publication Date:
Research Org.:
Ernest Orlando Lawrence Berkeley NationalLaboratory, Berkeley, CA (US)
Sponsoring Org.:
USDOE Director. Office of Science. Basic EnergySciences
OSTI Identifier:
932677
Report Number(s):
LBNL-59626
Journal ID: ISSN 1463-9076; R&D Project: 402303; BnR: KC0302010; TRN: US200813%%459
DOE Contract Number:  
DE-AC02-05CH11231
Resource Type:
Journal Article
Resource Relation:
Journal Name: Physical Chemistry Chemical Physics; Journal Volume: 9; Related Information: Journal Publication Date: 2007
Country of Publication:
United States
Language:
English
Subject:
37; CARBON DIOXIDE; CARBON MONOXIDE; CATALYSIS; CATALYSTS; HYDROGENATION; KINETICS; METHANE; RUTHENIUM; SPECTRA; SPECTROSCOPY; WATER

Citation Formats

Wasylenko, Walter, and Frei, Heinz. Time-Resolved FT-IR Spectroscopy of CO Hydrogenation overSupported Ru Catalyst at 700K. United States: N. p., 2006. Web.
Wasylenko, Walter, & Frei, Heinz. Time-Resolved FT-IR Spectroscopy of CO Hydrogenation overSupported Ru Catalyst at 700K. United States.
Wasylenko, Walter, and Frei, Heinz. Mon . "Time-Resolved FT-IR Spectroscopy of CO Hydrogenation overSupported Ru Catalyst at 700K". United States. doi:. https://www.osti.gov/servlets/purl/932677.
@article{osti_932677,
title = {Time-Resolved FT-IR Spectroscopy of CO Hydrogenation overSupported Ru Catalyst at 700K},
author = {Wasylenko, Walter and Frei, Heinz},
abstractNote = {Time-resolved FT-IR spectra of carbon monoxide hydrogenation over alumina-supported ruthenium were recorded on the millisecond timescale at 703 K using various H{sub 2} concentrations (1 atm total pressure). Adsorbed carbon monoxide was detected along with gas phase products methane (3016 and 1306 cm{sup -1}), water (sharp bands from 1900 - 1300 cm{sup -1}), and carbon dioxide (2348 cm{sup -1}). No other surface species were detected other than adsorbed carbon monoxide. The rate of formation of methane (2.5 {+-} 0.4 s{sup -1}) coincides with the rate of formation of carbon dioxide (3.4 {+-} 0.6 s{sup -1}), and bands due to water are observed to grow in over time. These results establish that methane and carbon dioxide originate from the same intermediate. The adsorbed carbon monoxide band is broad and unsymmetrical with a maximum at 2010 cm{sup -1} in spectra observed at 36 ms that shifts over 3000 ms to 1960 cm{sup -1} due to decreasing amounts of adsorbed carbon monoxide. Kinetic analysis of the adsorbed carbon monoxide band reveals that only a portion of the band can be temporally linked to gas phase products that we observe over the first 1000 ms of catalysis. This result suggests that we are observing dispersive kinetics, which is most likely due to heterogeneity of the surface environment.},
doi = {},
journal = {Physical Chemistry Chemical Physics},
number = ,
volume = 9,
place = {United States},
year = {Mon Feb 13 00:00:00 EST 2006},
month = {Mon Feb 13 00:00:00 EST 2006}
}