Enhanced Hydrogen Evolution in the Presence of Plasmonic Au-Photo-Sensitized g-C3N4 with an Extended Absorption Spectrum from 460 to 640 nm

Extensively spectral-responsive photocatalytic hydrogen production was achieved over g-C3N4 photo-sensitized by Au nanoparticles. The photo-sensitization, which was achieved by a facile photo-assisted reduction route, resulted in an extended spectral range of absorption from 460 to 640 nm. The photo-sensitized g-C3N4 (Au/g-C3N4) photocatalysts exhibit significantly enhanced photocatalytic hydrogen evolution with a TOF value of 223 μmol g-1 h-1, which is a 130-fold improvement over g-C3N4. The hydrogen production result confirms that Au nanoparticles are effective photo-sensitizers for the visible light-responsive substrate g-C3N4. UV-vis diffuse reflection spectra (DRS), photoluminescence spectra (PL), electron spin resonance (ESR), and electrochemical measurements were used to investigate the transfer process of photogenerated electrons. The optimal Au/g-C3N4 photocatalyst displays the lowest charge transfer resistance of 18.45 Ω cm-2 and a high electron transfer efficiency, as determined by electrochemical impedance spectroscopy (EIS). The photo-sensitized g-C3N4 shows a broad range of response to visible light (400-640 nm), with significantly high incident photon-to-current efficiency (IPCE) values of 14.52%, 2.9%, and 0.74% under monochromatic light irradiation of 400, 550, and 640 nm, respectively. ESR characterization suggests that Au nanoparticles are able to absorb visible light of wavelengths higher than 460 nm and to generate hot electrons due to the SPR effect.