Surface active oxygen engineering of photoanodes to boost photoelectrochemical water and alcohol oxidation coupled with hydrogen production

Photoelectrochemical conversion of solar energy into fuels (or chemicals) is in urgent need of efficient photoanodes to drive its practical applications. Nevertheless, the development of high performance photoanode usually suffers from slow charge transfer and sluggish surface catalytic kinetics. Here, we report a surface active oxygen engineering strategy through the modification and activation of NiCo layered double hydroxide (NiCo-LDH), where the activated NiCo-LDH (NiCo-LDH-Act) captures the photogenerated holes and acts as cocatalyst for surface oxidation reactions. The as-developed BiVO4/NiCo-LDH-Act achieves more than 3-fold higher photocurrent density than that of pristine BiVO4. Experimental integrated with theoretical studies further testify the bifunctional of NiCo-LDH-Act for hole transport and catalytic reactions. Moreover, the adsorbed ·OH originated from active oxygen enables efficient oxidation of glycerol to attain 1,3-dihydroxyacetone (DHA) with a productivity of 20.5 μmol cm–2 h–1 at 1.4 V vs. RHE with simultaneously producing hydrogen at the cathode.