Abstract

2D transition metal dichalcogenides (TMDs) are emerging as promising alternative electrocatalysts for hydrogen evolution reaction (HER). However, key challenges are the limited density of available activity sites and poor electron accessibility. Herein, Cu film supported MoS2-based electrocatalyst with partial 1T phase and 3D architecture is constructed by inkjet printing. We aim to investigate if this configuration could provide largely exposed edge sites and enhance electron transfer for ultra-efficient hydrogen production. Towards this end, an ink containing few-layer MoS2 nanosheets and reduced graphene oxide (RGO) is firstly prepared by liquid-phase exfoliation, in which semiconducting 2H-MoS2 is partially transformed to metallic 1 T-MoS2. We demonstrate that 1) nanosized few-layer MoS2 spatially patterned by inkjet-printing provides sufficient active site exposure, 2) the 1T-MoS2 and RGO conductive network reduce the charge-transfer impedance, and 3) the Cu support enhances the catalyst-electrode charge injection. Our all-in-one structure exhibits outstanding HER activities with low overpotential (51 mV at 10 mA cm−2 and 126 mV at 100 mA cm−2) and very low Tafel slope (32 mV dec-1). Also, the as-engineered electrode demonstrates ultrahigh cathodic current density. This work provides a facile, inexpensive, and scalable way for designing and fabricating TMDs-based electrocatalysts with excellent HER activity.

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