Iron-doping Accelerating NADH Oxidation over Carbon Nitride

doi:10.1007/s40242-020-0293-x

高等学校化学研究 ›› 2020, Vol. 36 ›› Issue (6): 1076-1082.doi: 10.1007/s40242-020-0293-x

Iron-doping Accelerating NADH Oxidation over Carbon Nitride

ZHANG Yuanyuan¹, HUANG Xiaohua¹, LI Jiashu¹, LIN Gang¹, LIU Wengang¹, CHEN Zupeng², 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

收稿日期:2020-09-01 修回日期:2020-10-17 出版日期:2020-12-01 发布日期:2020-12-03
通讯作者: LIU Jian E-mail:liujian@qust.edu.cn
基金资助:
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).

Iron-doping Accelerating NADH Oxidation over Carbon Nitride

ZHANG Yuanyuan¹, HUANG Xiaohua¹, LI Jiashu¹, LIN Gang¹, LIU Wengang¹, CHEN Zupeng², 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

Received:2020-09-01 Revised:2020-10-17 Online:2020-12-01 Published:2020-12-03
Contact: LIU Jian E-mail:liujian@qust.edu.cn
Supported by:
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).

摘要/Abstract

摘要： 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.

关键词: Cofactor regeneration, NADH oxidation, Photocatalysis, Carbon nitride, π-π interaction

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.

Key words: Cofactor regeneration, NADH oxidation, Photocatalysis, Carbon nitride, π-π interaction

ZHANG Yuanyuan, HUANG Xiaohua, LI Jiashu, LIN Gang, LIU Wengang, CHEN Zupeng, LIU Jian. Iron-doping Accelerating NADH Oxidation over Carbon Nitride[J]. 高等学校化学研究, 2020, 36(6): 1076-1082.

ZHANG Yuanyuan, HUANG Xiaohua, LI Jiashu, LIN Gang, LIU Wengang, CHEN Zupeng, LIU Jian. Iron-doping Accelerating NADH Oxidation over Carbon Nitride[J]. Chemical Research in Chinese Universities, 2020, 36(6): 1076-1082.

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Iron-doping Accelerating NADH Oxidation over Carbon Nitride

Iron-doping Accelerating NADH Oxidation over Carbon Nitride

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