Layered double hydroxide (LDH)-based photocatalysts have
attracted
more attention in photocatalysis due to their low cost, wide band
gaps, and adjustable photocatalytic active sites; however, their low
photogenerated carrier separation efficiency limits their photocatalytic
efficiency. Herein, a NiAl-LDH/Ni-doped Zn0.5Cd0.5S (LDH/Ni-ZCS) S-scheme heterojunction is rationally designed and
constructed from kinetically and thermodynamically favorable angles.
The 15% LDH/1% Ni-ZCS displays comparable photocatalytic hydrogen
evolution (PHE) activity with a rate of 6584.0 μmol g–1 h–1, which exceeds by ∼6.14- and ∼1.73-fold
those of ZCS and 1% Ni-ZCS, respectively, and outperforms most of
the previously reported LDH-based and metal sulfide-based photocatalysts.
In addition, the apparent quantum yield of 15% LDH/1% Ni-ZCS reaches
12.1% at 420 nm. In situ X-ray photoelectron spectroscopy,
photodeposition, and theoretical calculation reveal the specific transfer
path of photogenerated carriers. On this basis, we propose the possible
photocatalytic mechanism. The fabrication of the S-scheme heterojunction
not only accelerates the separation of photogenerated carriers but
also decreases the activation energy of H2 evolution and
improves the redox capacity. Moreover, there are huge amounts of hydroxyl
groups distributed on the surface of photocatalysts, which is highly
polar and easy to combine with H2O with a large dielectric
constant to form a hydrogen bond, which can further accelerate PHE.