Kalanur Shankara S, Lee Young Jae, Seo Hyungtak
Department of Materials Science and Engineering, Ajou University, Suwon 443-739, Republic of Korea.
Department of Energy Systems Research, Ajou University, Suwon 443-739, Republic of Korea.
ACS Appl Mater Interfaces. 2021 Jun 9;13(22):25906-25917. doi: 10.1021/acsami.1c03109. Epub 2021 May 27.
Exploring the ideal and stable semiconductor material for the efficient photoelectrochemical (PEC) overall water splitting reaction has remained a major challenge. Herein, we develop a facile hydrothermal method for the fabrication of monoclinic Pb[VO] and orthorhombic PbVO thin films for the efficient and stable PEC overall water splitting applications. Detailed characterization was performed to study the crystal structure and optical, electrical, and electrochemical properties. The band edge positions of Pb[VO] and PbVO are determined using spectroscopic data, revealing the conduction band edge positioned near the water reduction potential [∼0 V vs reversible hydrogen electrode (RHE)] and the valence band edge positioned well above the water oxidation potential, indicating the possible utilization of photogenerated electrons and holes for efficient water reduction and oxidation, respectively. With the optimized PbVO thin films, a maximum photocurrent of 0.35 mA cm was obtained at 1.23 V versus RHE and the stable production of both O and H is observed with >90% Faradaic efficiency. Importantly, this work demonstrates the possibility of utilizing lead vanadate materials for PEC water splitting applications.
探索用于高效光电化学(PEC)全水分解反应的理想且稳定的半导体材料一直是一项重大挑战。在此,我们开发了一种简便的水热法来制备单斜晶系的Pb[VO]和正交晶系的PbVO薄膜,用于高效且稳定的PEC全水分解应用。进行了详细的表征以研究晶体结构以及光学、电学和电化学性质。利用光谱数据确定了Pb[VO]和PbVO的带边位置,结果表明导带边位于析氢电位附近[相对于可逆氢电极(RHE)约为0 V],价带边位于析氧电位之上,这表明光生电子和空穴分别有可能用于高效的析氢和析氧反应。使用优化后的PbVO薄膜,在相对于RHE为1.23 V时获得了0.35 mA cm的最大光电流,并且观察到O和H的稳定产生,法拉第效率>90%。重要的是,这项工作证明了利用钒酸铅材料进行PEC水分解应用的可能性。