Simultaneous copper incorporation in core/shell-structured eco-friendly quantum dots for high-efficiency photoelectrochemical hydrogen evolution

The rational design of elemental incorporation in colloidal eco-friendly core/shell quantum dots (QDs) holds the potential to synergistically tailor their electronic band structure and carrier kinetics for applications in forthcoming "green" and high-efficiency solar energy conversion. Herein, we have conducted simultaneous Cu incorporation in both the core and shell regions of environment-benign AgInSe (AISe)/ZnSe core/shell QDs to realize high-efficiency solar-driven photoelectrochemical (PEC) hydrogen evolution. It is verified that Cu incorporation in AISe core enables an upward shift in the position of the band edge relative to the ZnSe shell, which promoted the electron delocalization and extended the lifetime of exciton. Simultaneously, Cu incorporation in the ZnSe shell further results in the trapping of photoinduced holes from AISe core, leading to a decelerated recombination of carriers. The prepared Cu-AISe/ZnSe:Cu QDs with optimized optoelectronic properties have been successfully employed to fabricate QDs-PEC devices, delivering a maximum photocurrent density of 9.1 mA cm-2 under standard AM 1.5 G illumination (100 mW cm-2). Our findings indicate that synchronous elemental incorporation in eco-friendly core/shell QDs is a promising strategy to achieve future high-performance solar-to-hydrogen conversion systems.