Photocatalytic hydrogen production of copolymers containing diiron model compounds in the presence of benzonitrile dye

Abstract

In this paper, a kind of azapropylene [FeFe]-hydrogenases model (1) containing styrene structure was synthesized by classical ammonia condensation reaction. Then, a series of new metallopolymers (2a/2b/2c) were synthesized by copolymerization of styrene group and 2-(Dimethylamino)ethyl methacrylate (DMAEMA) with different proportions. The precursor (1) and metallopolymers (2a/2b/2c) were characterized by NMR, GPC, XPS, FT-IR, ICP-MS and TG-DTA, and the contents of metal model substance in the metallopolymers (2a/2b/2c) were accurately determined. Subsequently, the photocatalytic hydrogen production performance of the catalysts were studied. The photocatalytic system consists of photosensitizer (2,4,5,6-Tetrakis (diphenylamino)-isophthalonitrile), solvent (DMF/H2O) and electron donor (NEt3). Under the optimized conditions, the maximum hydrogen production of the catalytic system can reach 0.704 mmol (1, 0.34 mg) and 0.812 mmol (2a, 10 mg) within 1 h. The catalysts still have certain catalytic activity after 30 h of photocatalytic reaction. During a catalytic time of up to 30 h, 2c had the highest TON, with a value of 24530. In addition, the effect of the polymerization ratio of precursor 1 to DMAEMA monomer in the metallopolymers (2a/2b/2c) on the catalytic efficiency was also studied.