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Probing the active sites of newly predicted stable Janus scandium dichalcogenides for photocatalytic water-splitting
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. Southwest Univ Sci & Technol, Stale Key Lab Environm Friendly Energy Mat, Natl Collaborat Innovat Ctr Nucl Waste & Environ, Mianyang 621010, Sichuan, Peoples R China. (Condensed Matter Theory Group)
Royal Inst Technol KTH, Appl Mat Phys, Dept Mat & Engn, S-10049 Stockholm, Sweden.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory. Royal Inst Technol KTH, Appl Mat Phys, Dept Mat & Engn, S-10049 Stockholm, Sweden. (Condensed Matter Theory Group)ORCID iD: 0000-0003-1231-9994
2019 (English)In: Catalysis Science & Technology, ISSN 2044-4753, E-ISSN 2044-4761, Vol. 9, no 18, p. 4981-4989Article in journal (Refereed) Published
Abstract [en]

The Janus structures of transition metal dichalcogenides with intrinsic dipoles have recently drawn attention as efficient candidates in the class of non-precious metal photocatalysts for water splitting. Here, we have proposed Janus ScXY (X/Y = S, Se, or Te, X not equal Y) monolayers as promising catalysts for the hydrogen evolution reaction (HER). We have thoroughly investigated the structural stabilities of the ScXY monolayers, as a primary step to understand the splitting mechanism more accurately. It has been observed that Janus ScSSe and ScSeTe monolayers are dynamically, thermally and mechanically stable, whereas the ScSTe monolayer is dynamically unstable. Moreover, based on hybrid functional (HSE06) calculations, these stable ScSSe and ScSeTe monolayers are semiconductors with direct band gaps of 1.810 and 0.921 eV, respectively. Considering spin-orbit coupling on top of the HSE06 calculations results in an insignificant change in the band gaps. The steady optical responses of Janus ScSSe and ScSeTe, respectively, in the visible and near IR spectra demonstrate their photocatalytic activities in the respective regions. Interestingly, we have observed excellent performance shown by the ScSeTe monolayer, where both surfaces are catalytically active, and maintain close to thermoneutral conditions with near-zero adsorption free energy at different H* coverages. Comparatively, the ScSSe monolayer shows poor performance for the HER due to strong bonds with the adsorbed hydrogen. Also, it has been confirmed that even the application of +/- 2% strain on the ScSSe monolayer does not enhance its HER activity. Our theoretical predictions demonstrate that out of all the Janus ScXY monolayers studied here, ScSeTe is the most active catalyst for the HER to efficiently split water, which certainly could make it worth performing further experimental investigations.

Place, publisher, year, edition, pages
ROYAL SOC CHEMISTRY , 2019. Vol. 9, no 18, p. 4981-4989
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-395844DOI: 10.1039/c9cy01014aISI: 000487788800012OAI: oai:DiVA.org:uu-395844DiVA, id: diva2:1365540
Funder
Swedish Research Council, 2016-06014Carl Tryggers foundation , 18.04Available from: 2019-10-25 Created: 2019-10-25 Last updated: 2019-10-25Bibliographically approved

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Ahuja, Rajeev

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