Iron-doping Accelerating NADH Oxidation over Carbon Nitride

Abstract

As a state-of-the-art conjugated polymer photocatalyst, graphitic carbon nitride(abbreviated as g-C₃N₄) has shown great potential in photocatalytic cofactor(reduced form of nicotinamide adenine dinucleotide, NADH) regeneration. Herein, Fe-doped g-C₃N₄ was engineered for photocatalytic NADH oxidation. The π-π interaction between the NADH molecule and the conjugated heptazine building block facilitates the adsorption of NADH onto the framework, as revealed by density functional theory(DFT) calculations. Furthermore, iron doping promoted the oxidation kinetics of NADH under blue LED illumination. The conversion ratio of NADH to its oxidized form could be up to 85.7% in 20 min, comparing with 59.4% for metal-free counterpart. Enzyme assay employing formate dehydrogenase(FDH) further verified the selectivity of the products, with 67.5%±2.6% of enzymatically active 1,4-NADH being regenerated following the oxidation process. Scavenger experiments suggest the dominant role of photo-induced electrons in the oxidation of NADH. This work could shed light on developing a novel cofactor regeneration route through the synergistic effect between the metal doping and noncovalent interaction based on the conjugated polymer.

Keywords

Cofactor regeneration / NADH oxidation / Photocatalysis / Carbon nitride / π-π interaction

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