Abstract

Scalable synthesis of 2D materials is a prerequisite for their commercial exploitation. Here, a novel method of producing nanocrystalline molybdenum disulfide (MoS2) at the liquid–liquid interface is demonstrated by decomposing a molecular precursor (tetrakis(N,N-diethyldithiocarbamato) molybdenum(IV)) in an organic solvent. The decomposition occurs over a few hours at room temperature without stirring or the addition of any surfactants, producing MoS2 which can be isolated onto substrates of choice. The formation of MoS2 at the liquid–liquid interface can be accelerated by the inclusion of hydroxide ions in the aqueous phase, which we propose to act as a catalyst. The precursor concentration was varied to minimize MoS2 thickness, and the organic solvent was chosen to optimize the speed and quality of formation. The kinetics of the MoS2 formation has been investigated, and a reaction mechanism has been proposed. The synthesis method is, to the best of our knowledge, the first reported room-temperature synthesis of transition-metal dichalcogenides, offering a potential solution to scalable 2D material production.

Highlights

  • Two-dimensional (2D) materials have been the focus of significant scientific interest since the discovery of graphene.[1]

  • Electron paramagnetic resonance (EPR) suggests the presence of Mo5+ in the MoL4 precursor (Figure S4), which suggests that some oxidation may occur in solution, the extent of which cannot be quantified from this data alone

  • We have shown for the first time that a molybdenum coordination complex decomposes to produce a thin film of few-layer MoS2, which to the best of our knowledge is the first reported bottom-up room-temperature synthesis route to transition-metal dichalcogenide (TMD)

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Summary

Introduction

Two-dimensional (2D) materials have been the focus of significant scientific interest since the discovery of graphene.[1]. Monolayer hexagonal MoS2 is a direct band gap semiconductor (∼1.9 eV), with strong photoluminescence, whereas its bulk counterpart has a smaller indirect band gap (∼1.2 eV).[6]

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