pH-Controlled assembly of [ZnW12O40]6−-based hybrids from a 0D dimer to a 2D network: synthesis, crystal structure, and photocatalytic performance in transformation of toluene into benzaldehyde

苯甲醛 多金属氧酸盐 选择性 光催化 化学 二聚体 晶体结构 光电流 单斜晶系 结晶学 催化作用 材料科学 有机化学 光电子学
作者
Ke-Ke Guo,Yanli Yang,Si-Meng Dong,Fengyan Li,Xin-Ye Jiang,Lin Xu
出处
期刊:Dalton Transactions [Royal Society of Chemistry]
卷期号:50 (46): 17308-17318 被引量:4
标识
DOI:10.1039/d1dt02618f
摘要

Polyoxometalate-based organic-inorganic hybrids have attracted considerable attention due to their fascinating structures and wide application prospects. In this work, using the same building blocks, ligands and metal ions (ZnW12O406-(ZnW12), 2,2'-bipyridine (2,2'-bipy), and Cu2+), we synthesized three new POM-based hybrids by controlling the pH values of the reaction systems. These three compounds {(Zn0.6(H2)0.4W12O40)[Cu(2,2'-bipy)(H2O)][Cu(2,2'-bipy)(H2O)2][Cu(2,2'-bipy)(H2O)3]}2·6H2O (1), (Me4N)2{ZnW12O40[Cu(2,2'-bipy)(H2O)][Cu(2,2'-bipy)(H2O)3]}·5H2O (2), and {(Zn0.5(H2)0.5W12O40)[Cu(2,2'-bipy)][Cu(2,2'-bipy)(H2O)][Cu(2,2'-bipy)(H2O)2]}·5H2O (3) have been structurally characterized by single-crystal X-ray diffraction. Compound 1 appears as a dimeric cluster structure, while compounds 2 and 3 appear as a 1D chain structure and a 2D network, respectively. The semiconducting properties of compounds 1-3 are different, which was demonstrated by band gap (Eg) and photocurrent response measurements. Compound 3 can efficiently catalyze the photooxidation of toluene to benzaldehyde with high selectivity using molecular oxygen as the oxidant component. Moreover, compound 3 was recycled and reused three times without significant degradation in conversion and selectivity. In addition, the mechanism of the photocatalytic reaction was also investigated.
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