Fe atoms trapped on graphene as a potential efficient catalyst for room-temperature complete oxidation of formaldehyde: a first-principles investigation

Handle URI:
http://hdl.handle.net/10754/625004
Title:
Fe atoms trapped on graphene as a potential efficient catalyst for room-temperature complete oxidation of formaldehyde: a first-principles investigation
Authors:
Guo, Huimin; Li, Min; Liu, Xin; Meng, Changgong; Linguerri, Roberto; Han, Yu ( 0000-0003-1462-1118 ) ; Chambaud, Gilberte
Abstract:
We investigated the oxidation of formaldehyde, one of the major indoor air pollutants, into CO2 and H2O over Fe atoms trapped in defects on graphene by first-principles based calculations. These trapped Fe atoms are not only stable to withstand interference from the reaction environments but are also efficient in catalyzing the reactions between coadsorbed O-2 and formaldehyde. The oxidation of formaldehyde starts with the formation of a peroxide-like intermediate and continues by its dissociation into. eta(1)-OCHO coadsorbed with an OH radical. Then, the adsorbed OCHO undergoes conformational changes and hydride transfer, leading to the formation of H2O and CO2. Subsequent adsorption of O2 or formaldehyde facilitates desorption of H2O and a new reaction cycle initiates. The calculated barriers for formation and dissociation of the peroxide-like intermediate are 0.43 and 0.40 eV, respectively, and those for conformation changes and hydride transfer are 0.47 and 0.13 eV, respectively. These relatively low barriers along the reaction path suggest the potential high catalytic performance of trapped Fe atoms for formaldehyde oxidation.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division
Citation:
Guo H, Li M, Liu X, Meng C, Linguerri R, et al. (2017) Fe atoms trapped on graphene as a potential efficient catalyst for room-temperature complete oxidation of formaldehyde: a first-principles investigation. Catal Sci Technol 7: 2012–2021. Available: http://dx.doi.org/10.1039/c7cy00307b.
Publisher:
Royal Society of Chemistry (RSC)
Journal:
Catal. Sci. Technol.
Issue Date:
24-Mar-2017
DOI:
10.1039/c7cy00307b
Type:
Article
ISSN:
2044-4753; 2044-4761
Sponsors:
This work was supported by the NSFC (21573034, 21373036 and 21103015), the Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (second phase, No: NSFC2015_65 and NSFC2015_66), the Fundamental Research Funds for the Central Universities (DUT15LK18, DUT14LK09 and DUT12LK14) and the Special Academic Partner GCR Program from the King Abdullah University of Science and Technology. X. L. would also like to thank the Universite Paris-Est for the visiting professorship. The supercomputer time was provided by the National Supercomputing Center in Guangzhou, China, the Supercomputing Core Laboratory at the King Abdullah University of Science and Technology and the High Performance Computing Center, Dalian University of Technology.
Additional Links:
http://pubs.rsc.org/en/Content/ArticleLanding/2017/CY/C7CY00307B#!divAbstract
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division

Full metadata record

DC FieldValue Language
dc.contributor.authorGuo, Huiminen
dc.contributor.authorLi, Minen
dc.contributor.authorLiu, Xinen
dc.contributor.authorMeng, Changgongen
dc.contributor.authorLinguerri, Robertoen
dc.contributor.authorHan, Yuen
dc.contributor.authorChambaud, Gilberteen
dc.date.accessioned2017-06-14T12:17:33Z-
dc.date.available2017-06-14T12:17:33Z-
dc.date.issued2017-03-24en
dc.identifier.citationGuo H, Li M, Liu X, Meng C, Linguerri R, et al. (2017) Fe atoms trapped on graphene as a potential efficient catalyst for room-temperature complete oxidation of formaldehyde: a first-principles investigation. Catal Sci Technol 7: 2012–2021. Available: http://dx.doi.org/10.1039/c7cy00307b.en
dc.identifier.issn2044-4753en
dc.identifier.issn2044-4761en
dc.identifier.doi10.1039/c7cy00307ben
dc.identifier.urihttp://hdl.handle.net/10754/625004-
dc.description.abstractWe investigated the oxidation of formaldehyde, one of the major indoor air pollutants, into CO2 and H2O over Fe atoms trapped in defects on graphene by first-principles based calculations. These trapped Fe atoms are not only stable to withstand interference from the reaction environments but are also efficient in catalyzing the reactions between coadsorbed O-2 and formaldehyde. The oxidation of formaldehyde starts with the formation of a peroxide-like intermediate and continues by its dissociation into. eta(1)-OCHO coadsorbed with an OH radical. Then, the adsorbed OCHO undergoes conformational changes and hydride transfer, leading to the formation of H2O and CO2. Subsequent adsorption of O2 or formaldehyde facilitates desorption of H2O and a new reaction cycle initiates. The calculated barriers for formation and dissociation of the peroxide-like intermediate are 0.43 and 0.40 eV, respectively, and those for conformation changes and hydride transfer are 0.47 and 0.13 eV, respectively. These relatively low barriers along the reaction path suggest the potential high catalytic performance of trapped Fe atoms for formaldehyde oxidation.en
dc.description.sponsorshipThis work was supported by the NSFC (21573034, 21373036 and 21103015), the Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (second phase, No: NSFC2015_65 and NSFC2015_66), the Fundamental Research Funds for the Central Universities (DUT15LK18, DUT14LK09 and DUT12LK14) and the Special Academic Partner GCR Program from the King Abdullah University of Science and Technology. X. L. would also like to thank the Universite Paris-Est for the visiting professorship. The supercomputer time was provided by the National Supercomputing Center in Guangzhou, China, the Supercomputing Core Laboratory at the King Abdullah University of Science and Technology and the High Performance Computing Center, Dalian University of Technology.en
dc.publisherRoyal Society of Chemistry (RSC)en
dc.relation.urlhttp://pubs.rsc.org/en/Content/ArticleLanding/2017/CY/C7CY00307B#!divAbstracten
dc.titleFe atoms trapped on graphene as a potential efficient catalyst for room-temperature complete oxidation of formaldehyde: a first-principles investigationen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalCatal. Sci. Technol.en
dc.contributor.institutionSchool of Chemistry, State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian, P. R. Chinaen
dc.contributor.institutionUniversité Paris-Est, Laboratoire Modélisation et Simulation Multi Echelle, MSME UMR 8208 CNRS, 5 bd Descartes, F-77454 Marne-la-Vallée, Franceen
kaust.authorHan, Yuen
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