Computational search for single-layer transition-metal dichalcogenide photocatalysts

Houlong Zhuang, Richard G. Hennig

Research output: Contribution to journalArticle

243 Citations (Scopus)

Abstract

Some of the members of the family of single-layer transition-metal dichalcogenides have recently received a lot of attention for their promising electronic properties, with potential applications in electronic devices. In this work, we focus on the stability of the dichalcogenides and determine their potential for photocatalytic water splitting. Using a first-principles design approach, we perform a systematic theoretical study of the dichalcogenides MX2 (M = Nb, Mo, Ta, W, Ti, V, Zr, Hf, and Pt; X = S, Se, and Te). First, we use a van der Waals functional to accurately calculate their formation energies. The results reveal that most MX2 have similar formation energies to those of single-layer MoS2 and WS2, implying the ease of mechanically exfoliating a single-layer MX2 from their layered bulk counterparts. Next, we use the many-body G0W0 approximation to obtain the band structures, finding that about half of the MX2 are semiconductors. We then calculate conduction and valence band edge positions by combining the bandgap center energies from the density-functional calculations and the G0W0 quasiparticle bandgaps. Comparing these band edge positions to the redox potentials of water, we identify that single-layer MoS2, WS2, PtS2, and PtSe2 are potential photocatalysts for water splitting. Furthermore, we find that PtSe2 undergoes a semimetal-to- semiconductor transition when the dimension is reduced from three dimensional to two dimensional. Finally, large solvation enthalpies of these four candidate photocatalysts suggest their stability in aqueous solution.

Original languageEnglish (US)
Pages (from-to)20440-20445
Number of pages6
JournalJournal of Physical Chemistry C
Volume117
Issue number40
DOIs
StatePublished - Oct 10 2013
Externally publishedYes

Fingerprint

Photocatalysts
Transition metals
transition metals
water splitting
Water
Energy gap
energy of formation
Semiconductor materials
Metalloids
Solvation
Valence bands
Conduction bands
Electronic properties
Band structure
Density functional theory
metalloids
Enthalpy
electronics
solvation
conduction bands

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry

Cite this

Computational search for single-layer transition-metal dichalcogenide photocatalysts. / Zhuang, Houlong; Hennig, Richard G.

In: Journal of Physical Chemistry C, Vol. 117, No. 40, 10.10.2013, p. 20440-20445.

Research output: Contribution to journalArticle

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