Using high-efficiency and low-cost catalyst to replace
noble metal
platinum for electrocatalytic hydrogen evolution reaction (HER) provides
a broad prospect for the development of renewable energy technology,
which is an important task yet to be solved. Herein, we proposed an
efficient doping–adsorption–pyrolysis strategy for constructing
a robust coupling catalyst composed of single-atom Co–N3 sites anchored on an N-doped carbon (N–C) layer and
encapsulated Co nanocrystals (NCs) to activate the interfacial water
for accelerating HER. Beneficial to the strong synergistic effect
of Co–N3 sites and Co NCs, the optimized CoNC‑SA/N*–C catalyst showed excellent HER activity
and stability in both acidic and alkaline electrolytes. In
situ attenuated total reflectance–surface-enhanced
infrared absorption spectroscopy revealed that the rigid interfacial
water layer of Co–N3 sites inhibited the transport
of H2O*/OH*, while Co NCs promoted the transport of H2O*/OH* and increased the amount of available H2O* on Co–N3 sites by disordering the rigid interfacial
water network. Theoretical calculation showed that the coupling interface
structure destroyed the rigid interfacial network, and Co NCs modified
the electronic structure of Co–N3 sites, which is
beneficial to H2O dissociation and H adsorption, thus accelerating
the HER process. This work opens up new avenues for the construction
of coupling catalysts from the atomic scale to activate the interfacial
water for boosting HER electrocatalysis.
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