Graduate School of Life and Environmental Sciences, University of Tsukuba, 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8577, Japan.
Research Center of Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan.
J Colloid Interface Sci. 2023 Sep;645:176-187. doi: 10.1016/j.jcis.2023.04.085. Epub 2023 Apr 25.
Defects engineering on photocatalysts such as oxygen vacancies (OVs) is an effective approach for improving photocatalytic hydrogen (H) evolution efficiency. In this study, OVs modified P/Ag/AgO/AgPO/TiO (PAgT) composite was successfully fabricated via a photoreduction process by controlling the ratio of PAgT to ethanol (16, 12, 8, 6 and 4 g·L) under simulated solar light irradiation for the first time. Characterization methods confirmed the presence of OVs in the modified catalysts. Meanwhile, the OVs amount and their effects on the light absorption ability, charge transfer rate, conduction band and H evolution efficiency of the catalysts were also investigated. The results indicated that the optimal OVs amount endowed OVs-PAgT-12 with the strongest light absorption, the fastest electron transfer rate and suitable band gap for H evolution, leading to the highest H yield (863 μmol·h·g) under solar light irradiation. Moreover, OVs-PAgT-12 exhibited a superior stability during cyclic experiment, indicating its great potential for practical application. Furthermore, a sustainable H evolution process was proposed based on a combination of sustainable bio-ethanol resource, stable OVs-PAgT, abundant solar energy and recyclable methanol. This study would provide new insights into the design of defects modified composite photocatalyst for enhanced solar-to-hydrogen conversion.
缺陷工程在光催化剂上,例如氧空位 (OVs),是提高光催化产氢效率的有效方法。在这项研究中,首次通过光还原过程,通过控制 P/Ag/AgO/AgPO/TiO (PAgT) 复合材料与乙醇的比例 (16、12、8、6 和 4 g·L),在模拟太阳光照射下成功制备了 OVs 修饰的 PAgT 复合材料。表征方法证实了改性催化剂中存在 OVs。同时,还研究了 OVs 的数量及其对催化剂的光吸收能力、电荷转移速率、导带和 H 产率的影响。结果表明,最佳的 OVs 数量使 OVs-PAgT-12 具有最强的光吸收、最快的电子转移速率和适宜的带隙,从而在太阳光照射下产生了最高的 H 产率 (863 μmol·h·g)。此外,在循环实验中,OVs-PAgT-12 表现出优异的稳定性,表明其在实际应用中有很大的潜力。此外,基于可持续的生物乙醇资源、稳定的 OVs-PAgT、丰富的太阳能和可回收甲醇的组合,提出了一种可持续的 H 产氢过程。本研究将为设计用于增强太阳能到氢气转化的缺陷修饰复合光催化剂提供新的思路。