Iron-doping Accelerating NADH Oxidation over Carbon Nitride
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doi: 10.1007/s40242-020-0293-x
Article
Iron-doping Accelerating NADH Oxidation over Carbon Nitride ZHANG Yuanyuan1#, HUANG Xiaohua1#, LI Jiashu1, LIN Gang1, LIU Wengang1, CHEN Zupeng2 and LIU Jian1* 1. College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, P. R. China; 2. College of Chemical Engineering, Nanjing Forestry University, Nanjing 210037, P. R. China 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) regene ration. 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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Introduction
cost-effective and inherently sustainable pathway for fulfilling such a purpose. Zhang and coworkers[13,14] have reported the oxidation of NADH driven by conjugated polymers under light irradiation. Especially, the promising conjugated polymer based nanogels with high efficiency and tunability were designed for the oxidation purpose[14]. g-C3N4 has emerged as an outstanding polymeric semiconductor candidate for cofactor regeneration recent years due to its extraordinary physiochemical properties and suitable band gap[15―17]. However, the intrinsic drawbacks derived from the conjugated quasi two dimensional π system still limited the photocatalytic activity of pristine g-C3N4, especially toward oxidation reactions[18―20]. Herein, two-dimensional Fe-doped g-C3N4 nanosheets (Fe/CN) were fabricated via a NaCl-assisted pyrolysis strategy. Theoretically, the density functional theory(DFT) calculation was employed to unravel the π-π stacking interaction between the conjugated heptazine of the g-C3N4 and NADH molecules. The adsorption of NADH molecules onto the heptazine of the carbon nitride matrix and the following electron transfer can be occurred through π-π stacking interactions[21,22]. Experimentally, Fe/CN was then applied for photocatalytic NADH oxidation under light illumination
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