Unravelling the essential difference between TiOx and AlOx interface layers on Ta3N5 photoanode for photoelectrochemical water oxidation

Abstract Tantalum nitride (Ta3N5) is a very promising photoanode material due to its narrow band gap (2.1 eV) and suitable band alignment for solar water splitting. However, it suffers from severe photocorrosion during water oxidation. In this work, it was found that surface passivation by AlOx and TiOx layers results in dramatically different PEC performance of Ta3N5 photoanode for water oxidation. The mechanism study indicates that the negative charges on AlOx can generate additional field to promote separation of photogenerated charges, while the positive charges on TiOx layer show the opposite effect. As a result, the Ta3N5 based photoanode modified with AlOx layer gives a high photocurrent of 12.5 mA cm−2 for 24 h at 1.23 V versus the reversible hydrogen electrode (RHE). Dynamic analysis implies that the hole extraction and transfer are significantly improved by the modification with the AlOx layer. This work reveals the importance of the charges on surface passivation layer in interface engineering of photoelectrodes.