Jiang Wenchao, Li Siyuan, Sui Qi, Gao Yujie, Li Fei, Xia Lixin, Jiang Yi
College of Chemistry, Liaoning University, Shenyang, Liaoning, 110036, China.
School of Chemical and Materials Science, University of Science and Technology of China, Hefei, Anhui, 230026, China.
Adv Sci (Weinh). 2024 Jan;11(2):e2305919. doi: 10.1002/advs.202305919. Epub 2023 Nov 20.
Regulating the interfacial charge transfer behavior between cocatalysts and semiconductors remains a critical challenge for attaining efficient photoelectrochemical water oxidation reactions. Herein, using bismuth vanadate (BiVO ) photoanode as a model, it introduces an Au binding bridge as holes transfer channels onto the surfaces of BiVO , and the cyano-functionalized cobalt cubane (Co O ) molecules are preferentially immobilized on the Au bridge due to the strong adsorption of cyano groups with Au nanoparticles. This orchestrated arrangement facilitates the seamless transfer of photogenerated holes from BiVO to Co O molecules, forming an orderly charge transfer pathway connecting the light-absorbing layer to reactive sites. An exciting photocurrent density of 5.06 mA cm at 1.23 V versus the reversible hydrogen electrode (3.4 times that of BiVO ) is obtained by the Co O @Au(A)/BiVO photoanode, where the surface charge recombination is almost completely suppressed accompanied by a surface charge transfer efficiency over 95%. This work represents a promising strategy for accelerating interfacial charge transfer and achieving efficient photoelectrochemical water oxidation reaction.
调控助催化剂与半导体之间的界面电荷转移行为仍然是实现高效光电化学水氧化反应的一项关键挑战。在此，以钒酸铋（BiVO₄）光阳极作为模型，引入金结合桥作为空穴转移通道至BiVO₄表面，并且由于氰基与金纳米颗粒的强吸附作用，氰基功能化的钴立方烷（Co₄O₄）分子优先固定在金桥上。这种精心安排的布局促进了光生空穴从BiVO₄到Co₄O₄分子的无缝转移，形成了一条将光吸收层连接到反应位点的有序电荷转移途径。通过Co₄O₄@Au(A)/BiVO₄光阳极在相对于可逆氢电极1.23 V时获得了令人兴奋的5.06 mA cm⁻²的光电流密度（是BiVO₄的3.4倍），其中表面电荷复合几乎被完全抑制，同时表面电荷转移效率超过95%。这项工作代表了一种加速界面电荷转移并实现高效光电化学水氧化反应的有前景的策略。
