Hole Storage Interfacial Regulation of Sb₂Se₃ Photocathode with Significantly Enhanced Photoelectrochemical...

Although interfacial engineering materials for antimony selenide (Sb₂Se₃) photocathodes have been intensively studied, most of the previous research has focused on the development of photogenerated electron transfer promoters. In this work, Sb₂Se₃ photocathodes are innovatively modified by using ferrihydrite (Fh), which has been widely used as a hole storage layer in photoanodes. After modifying Fh, the photocurrent density of the Sb₂Se₃ photocathode was increased from -0.27 to -1.6 mA cm^-2 at 0 V_RHE with the onset potential positive shift about 150 mV, and an impressive injection efficiency of 83.84% was achieved. The major contribution of Fh to the photoelectrochemical (PEC) performance enhancement was demonstrated by various characterization studies. The results show that the enhancement performance of PEC is largely attributed to the capture of back-migrating holes by Fh, the reduction of interfacial charge transfer resistance, and the significant increase in electrochemical active surface area (ECSA). This work presents new insights into the application of hole storage layers in Sb₂Se₃-based photocathodes.