Photoelectrochemical
(PEC) water splitting is a potential solution
for a low-carbon society and clean energy storage due to its ability
to produce hydrogen and oxygen. However, the slow oxidation half-reaction
of the process has limited its overall efficacy, necessitating the
development of an efficient photoanode. Colloidal CsPbBr3 nanocrystals (NCs) have been identified as promising candidates
due to their high light absorption and valence band position. However,
the presence of the electrical insulator, long-chain oleate molecules,
on the surface of the CsPbBr3 NCs has hindered efficient
charge carrier separation and transport. To solve this problem, short-chain
1,2-ethanedithiol (EDT) ligands were used to replace the oleate ligands
on the surface of the CsPbBr3 NCs through a solid-state
ligand exchange method. This resulted in a reduction of the nanocrystal
spacing and a cross-linking reaction, which improved the photogenerated
carrier separation and transport while still passivating the dangling
bonds on the CsPbBr3 NC surface. Ultimately, this led to
a remarkable photocurrent density of 3.34 mA cm–2 (1.23 VRHE), which was 5.2 times higher than that of
the pristine oleate-CsPbBr3 NC (0.64 mA cm–2)-based device. This work presents an efficient way of developing
inorganic lead halide perovskite colloidal nanocrystal-based photoanodes
through surface ligand engineering.