Hainan Provincial Key Laboratory of Fine Chemicals, College of Chemical Engineering and Technology, Hainan University, Haikou 570228, China.
Int J Mol Sci. 2023 Jul 5;24(13):11106. doi: 10.3390/ijms241311106.
-Re(2,2'-bipyridine)(CO)Cl] (denoted as ReCC) is an efficient molecule-catalyst with high selectivity in the photoreduction of CO to CO in a homogeneous system. However, the two major drawbacks of Re(I) complexes in the homogeneous system, easy degradation and difficult separation, seriously hinder its development in the field of industrial applications. In this paper, we designed and prepared two different Re-complex fixation systems (denoted as ReCC@TiO-5 wt% and ReCC-TiO-5 wt%) based on TiO gel via the sensitization method and sol-gel method, respectively. Compared with a pure ReCC complex, both of them exhibited excellent photocatalytic reduction activity. In particular, the sol-gel hybrid system (ReCC-TiO-5 wt%) displayed outstanding positive synergistic effects on the photocatalytic activity and the long durability of the photocatalytic process. A series of characterizations were carried out to explore the probable photocatalytic reduction process mechanism, which provides the theoretical basis and technical support for the Re complex fixation method.
[Re(2,2'-联吡啶)(CO)Cl](表示为 ReCC)是一种高效的分子催化剂,在均相体系中对 CO 的光还原具有高选择性。然而,Re(I) 配合物在均相体系中存在的两个主要缺点,即易降解和难分离,严重阻碍了其在工业应用领域的发展。在本文中,我们分别通过敏化法和溶胶-凝胶法,基于 TiO 凝胶设计并制备了两种不同的 Re 配合物固定体系(表示为 ReCC@TiO-5wt%和 ReCC-TiO-5wt%)。与纯 ReCC 配合物相比,它们均表现出优异的光催化还原活性。特别是,溶胶-凝胶杂化体系(ReCC-TiO-5wt%)对光催化活性和光催化过程的长期稳定性表现出显著的正协同效应。进行了一系列的表征来探究可能的光催化还原过程机制,这为 Re 配合物固定方法提供了理论依据和技术支持。