Unique reactivity of Fe nanoparticles-defective graphene composites toward NH x (x = 0, 1, 2, 3) adsorption: A first-principles study

Handle URI:
http://hdl.handle.net/10754/562021
Title:
Unique reactivity of Fe nanoparticles-defective graphene composites toward NH x (x = 0, 1, 2, 3) adsorption: A first-principles study
Authors:
Liu, Xin; Meng, Changgong; Han, Yu ( 0000-0003-1462-1118 )
Abstract:
We investigated the electronic structure of Fe nanoparticle-graphene composites and the impact of the interfacial interaction on NH x (x = 0, 1, 2, 3) adsorption by first-principles based calculations. We found that Fe 13 nanoparticles can be stabilized by the sp 2 dangling bonds on single vacancy graphene substrate with a binding energy up to -7.07 eV. This interaction not only deformed the carbon atoms around the defect and gave rise to the stability of the Fe nanoparticle against sintering, but also had significant impact on the adsorption of NH x that is related to the catalytic performance of these composites in NH 3 decomposition. Doping of the single vacancy graphene with N or B can finely tune the adsorption of NH x. Further analysis revealed that the calculated adsorption energies of NH x on these composites correlated well with the shift of the average d-band center of the Fe nanoparticles and they were around the peak of the activity-adsorption energy curve for NH 3 decomposition catalysts, especially when doped with B. The optimal adsorption of NH x on Fe nanoparticles deposited on boron-doped defective graphene suggests the possible high stability and superior catalytic performance of these composites in the low-temperature catalytic decomposition of NH 3. This journal is © 2012 the Owner Societies.
KAUST Department:
Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Nanostructured Functional Materials (NFM) laboratory
Publisher:
Royal Society of Chemistry
Journal:
Physical Chemistry Chemical Physics
Issue Date:
2012
DOI:
10.1039/c2cp42141k
Type:
Article
ISSN:
14639076
Sponsors:
This work was supported by the Special Academic Partner GCR Program from King Abdullah University of Science and Technology. X. L. would also thank NSFC (21103015, 20273012, and 11174045), the Chinese Scholarship Council (2009606533), the Fundamental Research Funds for the Central Universities (DUT11LK19, DUT12LK14) and the Key Laboratory of Coastal Zone Environmental Processes YICCAS (201203) for support.
Appears in Collections:
Articles; Advanced Membranes and Porous Materials Research Center; Physical Sciences and Engineering (PSE) Division; Chemical Science Program

Full metadata record

DC FieldValue Language
dc.contributor.authorLiu, Xinen
dc.contributor.authorMeng, Changgongen
dc.contributor.authorHan, Yuen
dc.date.accessioned2015-08-03T09:43:00Zen
dc.date.available2015-08-03T09:43:00Zen
dc.date.issued2012en
dc.identifier.issn14639076en
dc.identifier.doi10.1039/c2cp42141ken
dc.identifier.urihttp://hdl.handle.net/10754/562021en
dc.description.abstractWe investigated the electronic structure of Fe nanoparticle-graphene composites and the impact of the interfacial interaction on NH x (x = 0, 1, 2, 3) adsorption by first-principles based calculations. We found that Fe 13 nanoparticles can be stabilized by the sp 2 dangling bonds on single vacancy graphene substrate with a binding energy up to -7.07 eV. This interaction not only deformed the carbon atoms around the defect and gave rise to the stability of the Fe nanoparticle against sintering, but also had significant impact on the adsorption of NH x that is related to the catalytic performance of these composites in NH 3 decomposition. Doping of the single vacancy graphene with N or B can finely tune the adsorption of NH x. Further analysis revealed that the calculated adsorption energies of NH x on these composites correlated well with the shift of the average d-band center of the Fe nanoparticles and they were around the peak of the activity-adsorption energy curve for NH 3 decomposition catalysts, especially when doped with B. The optimal adsorption of NH x on Fe nanoparticles deposited on boron-doped defective graphene suggests the possible high stability and superior catalytic performance of these composites in the low-temperature catalytic decomposition of NH 3. This journal is © 2012 the Owner Societies.en
dc.description.sponsorshipThis work was supported by the Special Academic Partner GCR Program from King Abdullah University of Science and Technology. X. L. would also thank NSFC (21103015, 20273012, and 11174045), the Chinese Scholarship Council (2009606533), the Fundamental Research Funds for the Central Universities (DUT11LK19, DUT12LK14) and the Key Laboratory of Coastal Zone Environmental Processes YICCAS (201203) for support.en
dc.publisherRoyal Society of Chemistryen
dc.titleUnique reactivity of Fe nanoparticles-defective graphene composites toward NH x (x = 0, 1, 2, 3) adsorption: A first-principles studyen
dc.typeArticleen
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Centeren
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentNanostructured Functional Materials (NFM) laboratoryen
dc.identifier.journalPhysical Chemistry Chemical Physicsen
dc.contributor.institutionSchool of Chemistry, Dalian University of Technology, Dalian 116024, Chinaen
kaust.authorLiu, Xinen
kaust.authorHan, Yuen
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