Coating photoanodes with transition‐metal hydroxides (TMH) is a promising approach for improving photoelectrochemical (PEC) water oxidation. However, the present system still suffers from high charge recombination and sluggish surface reactions. Herein, effective charge separation is achieved at the same time as boosting the surface catalytic reaction for PEC water splitting through decoration of plasmon metal (Ag) in a semiconductor/TMH coupling system. The kinetic behavior at the semiconductor/TMH and TMH/electrolyte interfaces is systematically evaluated by employing intensity modulated photocurrent spectroscopy, scanning photoelectrochemical microscopy, and oxygen evolution reaction model. It is found that both charge transfer and surface catalysis dynamics are enhanced through local surface plasmon resonance of Ag nanoparticles. The as‐prepared BiVO4/Co(OH)x‐Ag exhibits remarkable activity (≈4.64 times) in PEC water splitting in comparison with pure BiVO4. Notably, this smart approach can be also applied to other TMH (Ni(OH)2), reflecting its universality. This work provides a guiding design method for solar energy conversion with the semiconductor‐TMH system.

A novel magnetic heterogeneous g-C 3 N 4 /a-Fe 2 O 3 /Fe 3 O 4 catalyst was successfully synthesized through a simple hydrothermal method. The structure, morphology, and optical properties of the catalyst were

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Detrimental charge recombination at photoanode/electrolyte junctions severely impedes photoelectrochemical (PEC) performance. The deposition of cobalt phosphate (CoPi) onto photoanodes is an efficient approach to achieve high PEC efficiency. However, achieving performances at the required remains a huge challenge, owing to the passivation effect of CoPi. In this study, function‐tunable strategy, whereby the passivation role is switched with the activation role, is exploited to modulate PEC performance through simultaneous activation of interface charge transfer and surface catalysis. By depositing nickel‐doped CoPi onto a BiVO4 (BV) substrate, the integrated system (BV/Ni1Co7Pi) exhibits a remarkable photocurrent density (4.15 mA cm−2), which is a 4.6‐fold increase relative to BV (0.90 mA cm−2). Moreover, the satisfactory performance can be also achieved on α‐Fe2O3 photoanode. These findings provide guidance for improving the efficiency of CoPi on photoanodes for PEC water oxidation.