Platinum
diselenide (PtSe2) is a group-10 two-dimensional
(2D) transition metal dichalcogenide that exhibits the most prominent
atomic-layer-dependent electronic behavior of “semiconductor-to-semimetal”
transition when going from monolayer to bulk form. This work demonstrates
an efficient photoelectrochemical (PEC) conversion for direct solar-to-hydrogen
(H2) production based on 2D layered PtSe2/Si
heterojunction photocathodes. By systematically controlling the number
of atomic layers of wafer-scale 2D PtSe2 films through
chemical vapor deposition (CVD), the interfacial band alignments at
the 2D layered PtSe2/Si heterojunctions can be appropriately
engineered. The 2D PtSe2/p-Si heterojunction
photocathode consisting of a PtSe2 thin film with a thickness
of 2.2 nm (or 3 atomic layers) exhibits the optimized band alignment
and delivers the best PEC performance for hydrogen production with
a photocurrent density of −32.4 mA cm–2 at
0 V and an onset potential of 1 mA cm–2 at 0.29
V versus a reversible hydrogen electrode (RHE) after post-treatment.
The wafer-scale atomic-layer controlled band engineering of 2D PtSe2 thin-film catalysts integrated with the Si light absorber
provides an effective way in the renewable energy application for
direct solar-to-hydrogen production.
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