Critical role of the semiconductor-electrolyte interface in photocatalytic performance for water-splitting reactions using Ta3N5 particles

Handle URI:
http://hdl.handle.net/10754/563712
Title:
Critical role of the semiconductor-electrolyte interface in photocatalytic performance for water-splitting reactions using Ta3N5 particles
Authors:
Nurlaela, Ela; Ould-Chikh, Samy ( 0000-0002-3486-0944 ) ; Harb, Moussab ( 0000-0001-5540-9792 ) ; Del Gobbo, Silvano; Aouine, Mimoun; Puzenat, Eric; Sautet, Philippe; Domen, Kazunari; Basset, Jean-Marie ( 0000-0003-3166-8882 ) ; Takanabe, Kazuhiro ( 0000-0001-5374-9451 )
Abstract:
Distinct photocatalytic performance was observed when Ta3N 5 was synthesized from commercially available Ta2O 5 or from Ta2O5 prepared from TaCl5 via the sol-gel route. With respect to photocatalytic O2 evolution with Ag+ as a sacrificial reagent, the Ta3N5 produced from commercial Ta2O5 exhibited higher activity than the Ta3N5 produced via the sol-gel route. When the Ta3N5 photocatalysts were decorated with Pt nanoparticles in a similar manner, the Ta3N5 from the sol-gel route exhibited higher photocatalytic hydrogen evolution activity from a 10% aqueous methanol solution than Ta3N5 prepared from commercial Ta2O5 where no hydrogen can be detected. Detailed surface and bulk characterizations were conducted to obtain fundamental insight into the resulting photocatalytic activities. The characterization techniques, including XRD, elemental analysis, Raman spectroscopy, UV-vis spectroscopy, and surface-area measurements, revealed only negligible differences between these two photocatalysts. Our thorough characterization of the surface properties demonstrated that the very thin outermost layer of Ta3N5, with a thickness of a few nanometers, consists of either the reduced state of tantalum (TaN) or an amorphous phase. The extent of this surface layer was likely dependent on the nature of precursor oxide surfaces. DFT calculations based on partially oxidized Ta3N4.83O0.17 and N deficient Ta3N4.83 consisting of reduced Ta species well described the optoelectrochemical properties obtained from the experiments. Electrochemical and Mott-Schottky analyses demonstrated that the surface layer drastically affects the energetic picture at the semiconductor-electrolyte interface, which can consequently affect the photocatalytic performance. Chemical etching of the surface of Ta3N5 particles to remove this surface layer unites the photocatalytic properties with the photocatalytic performance of these two materials. Mott-Schottky plots of these chemically etched Ta3N5 materials exhibited similar characteristics. This result suggests that the surface layer (1-2 nm) determines the electrochemical interface, which explains the different photocatalytic performances of these two materials. © 2014 American Chemical Society.
KAUST Department:
KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Solar and Photovoltaic Engineering Research Center (SPERC); Chemical Science Program; Catalysis for Energy Conversion (CatEC)
Publisher:
American Chemical Society (ACS)
Journal:
Chemistry of Materials
Issue Date:
26-Aug-2014
DOI:
10.1021/cm502015q
Type:
Article
ISSN:
08974756
Sponsors:
The research reported in this publication was supported by the King Abdullah University of Science and Technology (KAUST). We thank Dr. Violaine Mendez of the KAUST Catalysis Center for assistance with performing the elemental analyses.
Appears in Collections:
Articles; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC); Solar and Photovoltaic Engineering Research Center (SPERC)

Full metadata record

DC FieldValue Language
dc.contributor.authorNurlaela, Elaen
dc.contributor.authorOuld-Chikh, Samyen
dc.contributor.authorHarb, Moussaben
dc.contributor.authorDel Gobbo, Silvanoen
dc.contributor.authorAouine, Mimounen
dc.contributor.authorPuzenat, Ericen
dc.contributor.authorSautet, Philippeen
dc.contributor.authorDomen, Kazunarien
dc.contributor.authorBasset, Jean-Marieen
dc.contributor.authorTakanabe, Kazuhiroen
dc.date.accessioned2015-08-03T12:07:25Zen
dc.date.available2015-08-03T12:07:25Zen
dc.date.issued2014-08-26en
dc.identifier.issn08974756en
dc.identifier.doi10.1021/cm502015qen
dc.identifier.urihttp://hdl.handle.net/10754/563712en
dc.description.abstractDistinct photocatalytic performance was observed when Ta3N 5 was synthesized from commercially available Ta2O 5 or from Ta2O5 prepared from TaCl5 via the sol-gel route. With respect to photocatalytic O2 evolution with Ag+ as a sacrificial reagent, the Ta3N5 produced from commercial Ta2O5 exhibited higher activity than the Ta3N5 produced via the sol-gel route. When the Ta3N5 photocatalysts were decorated with Pt nanoparticles in a similar manner, the Ta3N5 from the sol-gel route exhibited higher photocatalytic hydrogen evolution activity from a 10% aqueous methanol solution than Ta3N5 prepared from commercial Ta2O5 where no hydrogen can be detected. Detailed surface and bulk characterizations were conducted to obtain fundamental insight into the resulting photocatalytic activities. The characterization techniques, including XRD, elemental analysis, Raman spectroscopy, UV-vis spectroscopy, and surface-area measurements, revealed only negligible differences between these two photocatalysts. Our thorough characterization of the surface properties demonstrated that the very thin outermost layer of Ta3N5, with a thickness of a few nanometers, consists of either the reduced state of tantalum (TaN) or an amorphous phase. The extent of this surface layer was likely dependent on the nature of precursor oxide surfaces. DFT calculations based on partially oxidized Ta3N4.83O0.17 and N deficient Ta3N4.83 consisting of reduced Ta species well described the optoelectrochemical properties obtained from the experiments. Electrochemical and Mott-Schottky analyses demonstrated that the surface layer drastically affects the energetic picture at the semiconductor-electrolyte interface, which can consequently affect the photocatalytic performance. Chemical etching of the surface of Ta3N5 particles to remove this surface layer unites the photocatalytic properties with the photocatalytic performance of these two materials. Mott-Schottky plots of these chemically etched Ta3N5 materials exhibited similar characteristics. This result suggests that the surface layer (1-2 nm) determines the electrochemical interface, which explains the different photocatalytic performances of these two materials. © 2014 American Chemical Society.en
dc.description.sponsorshipThe research reported in this publication was supported by the King Abdullah University of Science and Technology (KAUST). We thank Dr. Violaine Mendez of the KAUST Catalysis Center for assistance with performing the elemental analyses.en
dc.publisherAmerican Chemical Society (ACS)en
dc.titleCritical role of the semiconductor-electrolyte interface in photocatalytic performance for water-splitting reactions using Ta3N5 particlesen
dc.typeArticleen
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentSolar and Photovoltaic Engineering Research Center (SPERC)en
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentCatalysis for Energy Conversion (CatEC)en
dc.identifier.journalChemistry of Materialsen
dc.contributor.institutionUniv Lyon 2, IRCELYON, CNRS, UMR 5256, F-69626 Villeurbanne, Franceen
dc.contributor.institutionUniv Lyon, Ecole Normale Super Lyon, Chim Lab, CNRS, F-69364 Lyon 07, Franceen
dc.contributor.institutionUniv Tokyo, Dept Chem Syst Engn, Bunkyo Ku, Tokyo 1138656, Japanen
kaust.authorOuld-Chikh, Samyen
kaust.authorHarb, Moussaben
kaust.authorDel Gobbo, Silvanoen
kaust.authorBasset, Jean-Marieen
kaust.authorTakanabe, Kazuhiroen
kaust.authorNurlaela, Elaen
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