Synthesis of tantalum carbide and nitride nanoparticles using a reactive mesoporous template for electrochemical hydrogen evolution

Handle URI:
http://hdl.handle.net/10754/562531
Title:
Synthesis of tantalum carbide and nitride nanoparticles using a reactive mesoporous template for electrochemical hydrogen evolution
Authors:
Alhajri, Nawal Saad ( 0000-0001-5977-640X ) ; Yoshida, Hiroshi; Anjum, Dalaver H.; Garcia Esparza, Angel T. ( 0000-0002-4884-171X ) ; Kubota, Jun; Domen, Kazunari; Takanabe, Kazuhiro ( 0000-0001-5374-9451 )
Abstract:
Tantalum carbide and nitride nanocrystals were prepared through the reaction of a tantalum precursor with mesoporous graphitic (mpg)-C 3N4. The effects of the reaction temperature, the ratio of the Ta precursor to the reactive template (mpg-C3N4), and the selection of the carrier gas (Ar, N2 and NH3) on the resultant crystal phases and structures were investigated. The produced samples were characterized using powder X-ray diffraction (XRD), CHN elemental analyses, thermogravimetric analyses (TGA), nitrogen sorption, a temperature-programmed reaction with mass spectroscopy (MS), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). The results indicate that the different tantalum phases with cubic structure, TaN, Ta2CN, and TaC, can be formed under a flow of nitrogen when formed at different temperatures. The Ta3N5 phase with a Ta5+ oxidation state was solely obtained at 1023 K under a flow of ammonia, which gasified the C 3N4 template and was confirmed by detecting the decomposed gaseous products via MS. Significantly, the formation of TaC, Ta2CN, and TaN can be controlled by altering the weight ratio of the C 3N4 template relative to the Ta precursor at 1573 K under a flow of nitrogen. The high C3N4/Ta precursor ratio generally resulted in high carbide content rather than a nitride one, consistent with the role of mpg-C3N4 as a carbon source. Electrochemical measurements revealed that the synthesized nanomaterials were consistently able to produce hydrogen under acidic conditions (pH 1). The obtained Tafel slope indicates that the rate-determining step is the Volmer discharge step, which is consistent with adsorbed hydrogen being weakly bound to the surface during electrocatalysis. © 2013 The Royal Society of Chemistry.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Advanced Nanofabrication, Imaging and Characterization Core Lab; Chemical Science Program; Core Labs; Catalysis for Energy Conversion (CatEC)
Publisher:
Royal Society of Chemistry
Journal:
Journal of Materials Chemistry A
Issue Date:
2013
DOI:
10.1039/c3ta12984e
Type:
Article
ISSN:
20507488
Appears in Collections:
Articles; Advanced Nanofabrication, Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorAlhajri, Nawal Saaden
dc.contributor.authorYoshida, Hiroshien
dc.contributor.authorAnjum, Dalaver H.en
dc.contributor.authorGarcia Esparza, Angel T.en
dc.contributor.authorKubota, Junen
dc.contributor.authorDomen, Kazunarien
dc.contributor.authorTakanabe, Kazuhiroen
dc.date.accessioned2015-08-03T10:41:36Zen
dc.date.available2015-08-03T10:41:36Zen
dc.date.issued2013en
dc.identifier.issn20507488en
dc.identifier.doi10.1039/c3ta12984een
dc.identifier.urihttp://hdl.handle.net/10754/562531en
dc.description.abstractTantalum carbide and nitride nanocrystals were prepared through the reaction of a tantalum precursor with mesoporous graphitic (mpg)-C 3N4. The effects of the reaction temperature, the ratio of the Ta precursor to the reactive template (mpg-C3N4), and the selection of the carrier gas (Ar, N2 and NH3) on the resultant crystal phases and structures were investigated. The produced samples were characterized using powder X-ray diffraction (XRD), CHN elemental analyses, thermogravimetric analyses (TGA), nitrogen sorption, a temperature-programmed reaction with mass spectroscopy (MS), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM). The results indicate that the different tantalum phases with cubic structure, TaN, Ta2CN, and TaC, can be formed under a flow of nitrogen when formed at different temperatures. The Ta3N5 phase with a Ta5+ oxidation state was solely obtained at 1023 K under a flow of ammonia, which gasified the C 3N4 template and was confirmed by detecting the decomposed gaseous products via MS. Significantly, the formation of TaC, Ta2CN, and TaN can be controlled by altering the weight ratio of the C 3N4 template relative to the Ta precursor at 1573 K under a flow of nitrogen. The high C3N4/Ta precursor ratio generally resulted in high carbide content rather than a nitride one, consistent with the role of mpg-C3N4 as a carbon source. Electrochemical measurements revealed that the synthesized nanomaterials were consistently able to produce hydrogen under acidic conditions (pH 1). The obtained Tafel slope indicates that the rate-determining step is the Volmer discharge step, which is consistent with adsorbed hydrogen being weakly bound to the surface during electrocatalysis. © 2013 The Royal Society of Chemistry.en
dc.publisherRoyal Society of Chemistryen
dc.titleSynthesis of tantalum carbide and nitride nanoparticles using a reactive mesoporous template for electrochemical hydrogen evolutionen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentAdvanced Nanofabrication, Imaging and Characterization Core Laben
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentCore Labsen
dc.contributor.departmentCatalysis for Energy Conversion (CatEC)en
dc.identifier.journalJournal of Materials Chemistry Aen
dc.contributor.institutionDivision of Chemical Process Engineering, Faculty of Engineering, Hokkaido University, Sapporo 060-8628, Japanen
dc.contributor.institutionDepartment of Chemical System Engineering, University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japanen
dc.contributor.institutionElements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University Katsura, Kyoto 615-8520, Japanen
kaust.authorAnjum, Dalaver H.en
kaust.authorTakanabe, Kazuhiroen
kaust.authorAlhajri, Nawal Saaden
kaust.authorGarcia Esparza, Angel T.en
All Items in KAUST are protected by copyright, with all rights reserved, unless otherwise indicated.