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A highly active and stable electrocatalyst for hydrogen evolution is developed based on the in situ formation of MoS2 nanoparticles on mesoporous graphene foams (MoS2/MGF). Taking advantage of its high specific surface area and its interconnected conductive graphene skeleton, MGF provides a favorable microenvironment for the growth of highly dispersed MoS2 nanoparticles while allowing rapid charge transfer kinetics. The MoS2/MGF nanocomposites exhibit an excellent electrocatalytic activity for the hydrogen evolution reaction with a low overpotential and substantial apparent current densities. Such enhanced catalytic activity stems from the abundance of catalytic edge sites, the increase of electrochemically accessible surface area and the unique synergic effects between the MGF support and active catalyst. The electrode reactions are characterized by electrochemical impedance spectroscopy. A Tafel slope of ≈42 mV per decade is measured for a MoS2/MGF modified electrode, suggesting the Volmer‐Heyrovsky mechanism of hydrogen evolution.

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