Department of Chemistry, The University of Alabama in Huntsville, 301 Sparkman Drive, Huntsville, AL, 35899, USA.
Department of Physics and Astronomy, The University of Alabama in Huntsville, 301 Sparkman Drive, Huntsville, AL, 35899, USA.
Photosynth Res. 2020 Feb;143(2):143-153. doi: 10.1007/s11120-019-00668-z. Epub 2019 Sep 9.
Photocatalytic water splitting using solar energy for hydrogen production offers a promising alternative form of storable and clean energy for the future. To design an artificial photosynthesis system that is cost-effective and scalable, earth abundant elements must be used to develop each of the components of the assembly. To develop artificial photosynthetic systems, we need to couple a catalyst for proton reduction to a photosensitizer and understand the mechanism of photo-induced electron transfer from the photosensitizer to the catalyst that serves as the fundamental step for photocatalysis. Therefore, our work is focused on the study of light driven electron transfer kinetics from the quantum dot systems made with inorganic chalcogenides in the presence of Ni-based reduction catalysts. Herein, we report the synthesis and characterization of four Ni(II) complexes of tetradentate ligands with amine and pyridine functionalities (N2/Py2) and their interactions with CdTe quantum dots stabilized by 3-mercaptopropionic acid. The lifetime of the quantum dots was investigated in the presence of the Ni complexes and absorbance, emission and electrochemical measurements were performed to gain a deeper understanding of the photo-induced electron transfer process.
利用太阳能进行光催化水分解为未来提供了一种有前途的可存储、清洁的能源替代形式。为了设计出具有成本效益和可扩展性的人工光合作用系统，必须使用丰富的地球元素来开发组件的各个部分。为了开发人工光合作用系统，我们需要将质子还原催化剂与光敏剂相耦合，并了解作为光催化基本步骤的从光敏剂到催化剂的光诱导电子转移的机制。因此，我们的工作重点是研究在存在基于 Ni 的还原催化剂的情况下，由无机硫属化物制成的量子点体系中的光驱动电子转移动力学。在此，我们报告了四种具有胺和吡啶官能团（N2/Py2）的四齿配体的 Ni(II) 配合物的合成和表征，以及它们与 3-巯基丙酸稳定的 CdTe 量子点的相互作用。研究了量子点在 Ni 配合物存在下的寿命，并进行了吸收、发射和电化学测量，以更深入地了解光诱导电子转移过程。
