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Closser, Richard
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article
Atomic and Molecular Layer Deposition of Hybrid Mo–Thiolate Thin Films with Enhanced Catalytic Activity
Abstract
A synthetic route toward hybrid MoS2-based materials that combines the 2D bonding of MoS2 with 3D networking of aliphatic carbon chains is devised, leading to a film with enhanced electrocatalytic activity. The hybrid inorganic–organic thin films are synthesized by combining atomic layer deposition (ALD) with molecular layer deposition (MLD) using the precursors molybdenum hexacarbonyl and 1,2-ethanedithiol and characterized by in situ Fourier transform infrared spectroscopy, and the resultant material properties are probed by X-ray photoelectron spectroscopy, Raman spectroscopy, and grazing incidence X-ray diffraction. The process exhibits a growth rate of 1.3 Å per cycle, with an ALD/MLD temperature window of 155–175 °C. The hybrid films are moderately stable for about a week in ambient conditions, smooth (σRMS ≈ 5 Å for films 60 Å thick) and uniform, with densities ranging from 2.2–2.5 g cm−3. The material is both optically transparent and catalytically active for the hydrogen evolution reaction (HER), with an overpotential (294 mV at −10 mA cm−2) superior to that of planar MoS2. The enhancement in catalytic activity is attributed to the incorporation of organic chains into MoS2, which induces a morphological change during electrochemical testing that increases surface area and yields high activity HER catalysts without the need for deliberate nanostructuring.