Department of Chemical, Materials and Industrial Production Engineering, University of Naples "Federico II", p.le V. Tecchio 80, 80125 Napoli, Italy.
CSGI, Center for Colloid and Interface Science, via della Lastruccia 3, 50019 Sesto Fiorentino, Italy.
Int J Mol Sci. 2023 Jan 19;24(3):2004. doi: 10.3390/ijms24032004.
The existing literature survey reports rare and conflicting studies on the effect of the preparation method of metal-based semiconductor photocatalysts on structural/morphological features, electronic properties, and kinetics regulating the photocatalytic H generation reaction. In this investigation, we compare the different copper/titania-based photocatalysts for H generation synthesized via distinct methods (i.e., photodeposition and impregnation). Our study aims to establish a stringent correlation between physicochemical/electronic properties and photocatalytic performances for H generation based on material characterization and kinetic modeling of the experimental outcomes. Estimating unknown kinetic parameters, such as charge recombination rate and quantum yield, suggests a mechanism regulating charge carrier lifetime depending on copper distribution on the TiO surface. We demonstrate that H generation photoefficiency recorded over impregnated CuO/TiO is related to an even distribution of Cu(0)/Cu(I) on TiO, and the formation of an Ohmic junction concertedly extended charge carrier lifetime and separation. The outcomes of the kinetic analysis and the related modeling investigation underpin photocatalyst physicochemical and electronic properties. Overall, the present study lays the groundwork for the future design of metal-based semiconductor photocatalysts with high photoefficiencies for H evolution.
现有文献调查报告表明，关于金属基半导体光催化剂的制备方法对结构/形态特征、电子性质以及调节光催化 H 生成反应动力学的影响的研究很少且相互矛盾。在这项研究中，我们比较了通过不同方法（即光沉积和浸渍）合成的用于 H 生成的不同铜/二氧化钛基光催化剂。我们的研究旨在通过对实验结果进行材料表征和动力学建模，在基于物质的物理化学/电子性质和光催化 H 生成性能之间建立严格的相关性。估计未知的动力学参数，例如电荷复合率和量子产率，表明电荷载流子寿命的调节机制取决于 Cu 在 TiO 表面的分布。我们证明，浸渍 CuO/TiO 上记录的 H 生成光电效率与 TiO 上 Cu(0)/Cu(I)的均匀分布以及协同扩展电荷载流子寿命和分离的欧姆结的形成有关。动力学分析的结果和相关的建模研究为光催化剂的物理化学和电子性质提供了依据。总的来说，本研究为未来设计具有高 H 演化光效的金属基半导体光催化剂奠定了基础。
