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Bismuth vanadate (BiVO4) is a promising photoanode material for efficient photoelectrochemical (PEC) water splitting, whereas its performance is inhibited by detrimental surface states. To solve the problem, herein, a low-cost organic molecule 1,3,5-benzenetricarboxylic acid (BTC) is selected for surface passivation of BiVO4 photoanodes (BVOs), which also provides bonding sites for Co2+ to anchor, resulting in a Co-BTC-BVO photoanode. Owing to its strong coordination with metal ions, BTC not only passivates surface states of BVO, but also provides bonding between BVO and catalytic active sites (Co2+) to form a molecular cocatalyst. Computational study and interfacial charge kinetic investigation reveal that chemical bonding formed at the interface greatly suppresses charge recombination and accelerates charge transfer. The obtained Co-BTC-BVO photoanode exhibits a photocurrent density of 4.82 mA/cm2 at 1.23 V vs. reversible hydrogen electrode (RHE) and a low onset potential of 0.22 VRHE under AM 1.5 G illumination, which ranks among the best photoanodes coupled with Co-based cocatalysts. This work presents a novel selection of passivation layers and emphasizes the significance of interfacial chemical bonding for the construction of efficient photoanodes.
The authors kindly acknowledge the financial support from the National Natural Science Foundation of China (No. 51672173, U1733130); Shanghai Science and Technology Committee (Nos. 21ZR1435700, 18520744700, and 18JC1410500); and Shanghai Jiao Tong University Medical Engineering Cross Research Program (No. YG2023ZD18). The computations in this paper were run on the Siyuan-1 cluster supported by the Center for High Performance Computing at Shanghai Jiao Tong University.