Photoelectrochemical
(PEC) water splitting over TiO2 photoanodes is a promising
strategy for hydrogen production due
to its eco-friendly, energy-saving, and low-cost nature. However,
the intrinsic drawbacks of TiO2, i.e.,
the too wide band gap and rapid exciton recombination, significantly
limit further enhancement of its performance. Herein, we report a
TiO2 nanotube array (TNA), which is implanted by Cu ions
and decorated by polymeric carbon nitride (PCN) nanosheets, as a photoanode
for the high-efficiency PEC water splitting. In such designed material,
Cu-ion implantation can effectively tailor the electronic structure
of TiO2, thus narrowing the band gap and enhancing the
electronic conductivity. Meanwhile, the PCN decoration induces TiO2/PCN heterojunctions, enhancing the visible light absorption
and accelerating the exciton separation. Upon this synergistic effect,
the modified TNA photoanode shows significantly improved PEC capability.
Its photocurrent density, solar-to-hydrogen efficiency, and applied
bias photon-to-current efficiency achieve 1.89 mA cm–2 at 1.23 VRHE (V vs reversible hydrogen
electrode), 2.31%, and 1.20% at 0.46 VRHE, respectively.
Importantly, this modified TNA supported on a meshlike Ti substrate
can be readily integrated with a perovskite solar cell to realize
unassisted PEC water splitting.