The
main challenge in water electrolysis, an appealing technique
to alleviate future energy crisis, is the design of efficient electrocatalysts
for hydrogen evolution reaction (HER). On the basis of an interface
self-assembly approach, we synthesize mesoporous nitrogen-doped carbon/Mo2C/reduced graphene oxide nanohybrids (denoted as mNC-Mo2C@rGO), which represent a new type of two-dimensional Mo2C/carbon hybrid nanomaterials and possess a sandwichlike structure
with well-defined mesopores. The method involves the co-self-assembly
of spherical micelles formed from polystyrene-block-poly(ethylene oxide), pyrrole (Py) monomers, and molybdate ions
(Mo7O24
6–) on GO surfaces
in aqueous solution, followed by polymerization of Py and calcination
of the nanocomposites at 900 °C under nitrogen atmosphere. The
resultant mNC-Mo2C@rGO nanosheets possess high N contents,
large specific surface areas (SSAs), and 4 nm Mo2C particles
well-distributed in the mesoporous carbon matrix. The Mo2C content is controllable in the range of 18.4–42.4 wt % by
adjusting the feed amount of Mo7O24
6–. In particular, mNC-Mo2C@rGO with an SSA of 344 m2/g and a Mo2C content of ca. 28 wt % exhibits the
highest HER catalytic activity in 1 M KOH electrolyte, with a 95 mV
overpotential at 10 mA/cm2, a Tafel slope of 49.8 mV/dec,
and a long-term stability of 60 h at 20 mA/cm2. This study
blazes a trail for the synthesis of new functional nanomaterials with
potential applications as efficient HER electrocatalysts.