We herein demonstrate the unusual effectiveness of two strategies in combination to enhance photoelectrochemical water splitting. First, the work function adjustment via molybdenum (Mo) doping significantly reduces the interfacial energy loss and increases the open-circuit photovoltage of bismuth vanadate (BiVO
4
) photoelectrochemical cells. Second, the creation and optimization of the heterojunction of boron (B) doping carbon nitride (C
3
N
4
) and Mo doping BiVO
4
to enforce directional charge transfer, accomplished by work function adjustment via B doping for C
3
N
4
, substantially boost the charge separation of photo-generated electron-hole pairs at the B-C
3
N
4
and Mo-BiVO
4
interface. The synergy between the above efforts have significantly reduced the onset potential, and enhanced charge separation and optical properties of the BiVO
4
-based photoanode, culminating in achieving a record applied bias photon-to-current efficiency of 2.67% at 0.54 V vs. the reversible hydrogen electrode. This work sheds light on designing and fabricating the semiconductor structures for the next-generation photoelectrodes.
High-temperature activation has been commonly used to boost the photoelectrochemical (PEC) performance of hematite nanowires for water oxidation, by inducing Sn diffusion from fluorine-doped tin oxide (FTO) substrate into hematite. Yet, hematite nanowires thermally annealed at high temperature suffer from two major drawbacks that negatively affect their performance. First, the structural deformation reduces light absorption capability of nanowire. Second, this "passive" doping method leads to nonuniform distribution of Sn dopant in nanowire and limits the Sn doping concentration. Both factors impair the electrochemical properties of hematite nanowire. Here we demonstrate a silica encapsulation method that is able to simultaneously retain the hematite nanowire morphology even after high-temperature calcination at 800 °C and improve the concentration and uniformity of dopant distribution along the nanowire growth axis. The capability of retaining nanowire morphology allows tuning the nanowire length for optimal light absorption. Uniform distribution of Sn doping enhances the donor density and charge transport of hematite nanowire. The morphology and doping engineered hematite nanowire photoanode decorated with a cobalt oxide-based oxygen evolution reaction (OER) catalyst achieves an outstanding photocurrent density of 2.2 mA cm at 0.23 V vs Ag/AgCl. This work provides important insights on how the morphology and doping uniformity of hematite photoanodes affect their PEC performance.
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