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Iron-doping Accelerating NADH Oxidation over Carbon Nitride

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Chemical Research in Chinese Universities Aims and scope

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.

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Author notes

  1. These authors contributed equally to this work.

Authors and Affiliations

  1. College of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao, 266042, P. R. China

    Yuanyuan Zhang, Xiaohua Huang, Jiashu Li, Gang Lin, Wengang Liu & Jian Liu

  2. College of Chemical Engineering, Nanjing Forestry University, Nanjing, 210037, P. R. China

    Zupeng Chen

Authors
  1. Yuanyuan Zhang
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  2. Xiaohua Huang
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  3. Jiashu Li
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  4. Gang Lin
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  5. Wengang Liu
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  6. Zupeng Chen
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  7. Jian Liu
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Corresponding author

Correspondence to Jian Liu.

Additional information

Supported by the Distinguished Young Scholar Fund of Natural Science Foundation of Shandong Province, China (No. ZR2019JQ05), the Key Basic Research Project of the Natural Science Foundation of Shandong Province, China (No. ZR2019ZD47) and the Fund of the Education Department of Shandong Province, China(No.2019KJC006).

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Zhang, Y., Huang, X., Li, J. et al. Iron-doping Accelerating NADH Oxidation over Carbon Nitride. Chem. Res. Chin. Univ. 36, 1076–1082 (2020). https://doi.org/10.1007/s40242-020-0293-x

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  • DOI: https://doi.org/10.1007/s40242-020-0293-x

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