Abstract
Large research efforts have been devoted to optimizing the output of earth-abundant photoabsorbers in solar-to-fuel (S2F) devices. Here, we report a Cu2O/Ga2O3 heterojunction/Si microwire photocathode with an underlying buried radial Si p–n junction, which achieves efficient light harvesting across the visible spectrum to over 600 nm, reaching an external quantum yield for hydrogen generation close to 80%, with a photocurrent onset above +1.35 V vs RHE, a photocurrent density of ∼10 mA/cm2 at 0 V vs RHE, and an ideal regenerative efficiency of 5.51%. We show step-by-step the effects of every photocathode design element (i.e., Si p–n junction, Cu2O layer thickness, microwire length, microwire pitch, etc.) on the overall efficiency of our final microwire Si/Cu2O photocathode by comparing every addition to a baseline Cu2O photocathode. Lastly, we show a stable operation exceeding 200 h at a bias potential of +1.0 V vs RHE, with an average current density of 4.5 mA/cm2.
Vijselaar, Wouter