Synthesis and photocatalytic activity of two different hydrogenase models based on DMAEMA copolymer structure

Abstract

In this paper, the copolymers (3/3a, 4/4a) of styrene phosphine derivatives (1, 2) and DMAEMA(Dimethylaminoethyl methacrylate) were synthesized by free radical polymerization. On this basis, two phosphine ligand substituted hydrogenase models were further synthesized. They were 5/5a containing different proportions of PNP{N[P(C6H5)2]2} ligands and 6/6a containing different proportions of PCP{N[CH2P(C6H5)2]2} ligands. The newly synthesized model compounds have good solubility in various solvents. The intermediates and final products were characterized by NMR, GPC, EDX, XPS, FT-IR, ICP-MS and TG-DTA. The photocatalytic performances of the catalysts were studied. Under the preferred conditions, the turnover numbers were 75(5a) and 113(6a) for catalysts in an hour of illumination. Under the same conditions, the photocatalytic efficiency of the catalysts were significantly better than that of similar small molecule or supported hydrogenase models reported in other literatures. In addition, a possible photocatalytic mechanism was proposed.