The electronic properties of electrode materials play a crucial role in defining their electrochemical behavior in energy conversion and storage devices. The assembly of van der Waals heterostructures and fabrication into mesoscopic devices enable the dependence of an electrochemical response on electronic properties to be systematically interrogated. Here, we evaluate the effect of charge carrier concentration on heterogeneous electron transfer at few-layer MoS 2 electrodes by combining spatially resolved electrochemical measurements with field-effect electrostatic manipulation of band alignment. Steady-state cyclic voltammograms and finiteelement simulations reveal a strong modulation of the measured electrochemical response for outer-sphere charge transfer at the electrostatic gate voltage. In addition, spatially resolved voltammetric responses, obtained at a series of locations at the surface of few-layer MoS 2 , reveal the governing role of in-plane charge transport on the electrochemical behavior of 2D electrodes, especially under conditions of low carrier densities.

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