cs9b03184_si_001.pdf (1.34 MB)
TaS2, TaSe2, and Their Heterogeneous Films as Catalysts for the Hydrogen Evolution Reaction
journal contribution
posted on 2020-02-21, 21:49 authored by Leyla Najafi, Sebastiano Bellani, Reinier Oropesa-Nuñez, Beatriz Martín-García, Mirko Prato, Lea Pasquale, Jaya-Kumar Panda, Petr Marvan, Zdeněk Sofer, Francesco BonaccorsoMetallic
two-dimensional transition-metal dichalcogenides (TMDs)
of the group 5 metals are emerging as catalysts for an efficient
hydrogen evolution reaction (HER). The HER activity of the group 5
TMDs originates from the unsaturated chalcogen edges and the highly
active surface basal planes, whereas the HER activity of the widely
studied group 6 TMDs originates solely from the chalcogen- or metal-unsaturated
edges. However, the batch production of such nanomaterials and their
scalable processing into high-performance electrocatalysts is still
challenging. Herein, we report the liquid-phase exfoliation of the
2H-TaS2 crystals by using 2-propanol to produce single/few-layer
(1H/2H) flakes, which are afterward deposited as catalytic films.
A thermal treatment-aided texturization of the catalytic films is
used to increase their porosity, promoting the ion access to the basal
planes of the flakes, as well as the number of catalytic edges of
the flakes. The hybridization of the H-TaS2 flakes and
H-TaSe2 flakes tunes the Gibbs free energy of the adsorbed
atomic hydrogen onto the H-TaS2 basal planes to the optimal
thermo-neutral value. In 0.5 M H2SO4, the heterogeneous
catalysts exhibit a low overpotential (versus RHE, reversible hydrogen
electrode) at the cathodic current of 10 mA cm–2 (η10) of 120 mV and high mass activity of 314 A
g–1 at an overpotential of 200 mV. In 1 M KOH, they
show a η10 of 230 mV and a mass activity of 220 A
g–1 at an overpotential of 300 mV. Our results provide
new insight into the usage of the metallic group 5 TMDs for the HER
through scalable material preparation and electrode processing.
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H-TaS 2 flakesscalable material preparationgroup 5 TMDsRHEHER activityHydrogen Evolution Reaction Metallicelectrodeoverpotentialmass activityH-TaSe 2 flakes tunessurface basal planeshydrogen evolution reaction2 H-TaS 2 crystalsH-TaS 2 basal planesmVcatalyst0.5 M H 2group 5 metalsfilmchalcogengroup 6 TMDs1 M KOH
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