Cu2O has great potential as a photocathode for photoelectrochemical
water splitting, and efficient charge separation through interface
modulation is the key for potential application. In this work, we
develop a facial strategy to maximally reduce the recombination of
charge carriers via CuSCN in two directions, that is, E-CuSCN on an
FTO substrate from ethylenediaminetetraacetic acid (EDTA) electrolyte
as the hole-transport layer and D-CuSCN on the Cu2O layer
from diethanolamine (DEA) electrolyte as the hole-storage layer. As
a result, the E-CuSCN/Cu2O/D-CuSCN with efficient charge
separation shows improved activity with a photocurrent density up
to 5 mA·cm–2, which is 7 times higher than
that of the pristine Cu2O. This work provides a new method
for separating photocharges based on the design of interfacial crystal
structure for high-efficiency photocathodes.