Hydrogen generation through photoelectrochemical (PEC) technology is one of the most appropriate ways for delivering sustainable fuel. Simultaneously, anisotropic properties will be exhibited by the materials with low crystal symmetry, allowing the tuning of the PEC properties by controlling the crystallographic orientation and exposed facets. Therefore, we synthesized copper tungstate films (CuWO) with highly exposed (100) crystal facets by regulating anions in the precursor solution. According to experimental characterization and density functional theory calculations, the CuWO film with a high exposure ratio of the (100) crystal facet has promoted charge transport with trap-free mode and reduced recombination of electrons and holes. Meanwhile, the oxygen evolution reaction is promoted on the (100) facet because of the relatively low energy barrier. Compared to the CuWO with other mixed exposure facets, CuWO with a highly exposed (100) facet presents a twofold current density (0.38 mA/cm) and one-fifteenth electron transit time (0.698 ms) and also has great stability (more than 6 h). These results provide an easy way to enhance the PEC performance by modulating the exposure facets of the film electrode.
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