A graphitic carbon nitride nanostructure has been successfully functionalized by incorporation of different silver contents and subsequent modification with an α-rich protein, namely hemoglobin. Mechanochemistry has been employed, as an efficient and sustainable procedure, for the incorporation of the protein. A complete characterization analysis has been performed following a multitechnique approach. Particularly, XPS data exhibited considerable differences in the C 1s region for the Hb/xAg@CN, ensuring the successful protein anchorage on the surface of the graphitic carbon nitride-based materials. The as-synthesized nanomaterials delivered impressive performance toward hydrogen evolution reactions with an overpotential of 79 mV at a current density of 10 mA/cm2 for Hb/20Ag@CN nanohybrids, which is comparable with the most efficient HER electrocatalysts reported in the literature. The outstanding HER properties were associated with the unique synergistic interactions, quantitatively measured, between AgNPs, Hb tertiary architecture, and the graphitic carbon nitride networks.
Keywords: bioconjugates; electrocatalysis; graphitic carbon nitride; hemoglobin; hydrogen evolution reaction; mechanochemistry; silver nanoparticles; synergy.