Unraveling and Manipulating of NADH Oxidation by Photogenerated Holes,ACS Catalysis

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Unraveling and Manipulating of NADH Oxidation by Photogenerated Holes
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-04-08 , DOI: 10.1021/acscatal.0c00471
Shaohua Zhang _{1,

2} , Jiafu Shi _{3,

4,

5} , Yixuan Chen ₁ , Qian Huo _{1,

2} , Weiran Li ₃ , Yizhou Wu _{1,

2} , Yiying Sun _{1,

2} , Yishan Zhang _{1,

2} , Xiaodong Wang ₆ , Zhongyi Jiang _{1,

2,

4,

5}

Affiliation

Photoenzymatic coupled catalysis, integrating semiconductor photocatalysis and enzymatic catalysis, exhibits great potential for light-driven synthesis. To make a photocatalyst and an enzyme act concertedly, nicotinamide-based cofactors have been widely used as an electron carrier. However, these cofactors are easily oxidized into an enzymatically inactive form by photogenerated holes. Herein, the oxidation mechanism of NADH, one typical nicotinamide-based cofactor, by photogenerated holes was reported. With CdS, g-C₃N₄ , and BiVO₄ as hole generators, NADH is oxidized into NAD⁺ or fragmented into ADP-ribose derivatives through a multistep electron transfer. Importantly, the fragmentation reaction is inhibited with dopamine and neutral red to coordinate electron transfer between NADH and photogenerated holes.

中文翻译：

解开和操纵光生空穴对NADH的氧化作用

结合了半导体光催化和酶催化的光酶偶联催化，显示出光驱动合成的巨大潜力。为了使光催化剂和酶协同作用，基于烟酰胺的辅因子已被广泛用作电子载体。但是，这些辅因子很容易被光生空穴氧化成酶活性形式。在此，报道了一种典型的基于烟酰胺的辅因子NADH被光生空穴的氧化机理。使用CdS，gC ₃ N ₄和BiVO ₄作为空穴发生剂，NADH被氧化成NAD ⁺或通过多步电子转移将其片段化为ADP-核糖衍生物。重要的是，碎裂反应被多巴胺和中性红抑制，以协调NADH和光生空穴之间的电子转移。

更新日期：2020-04-08

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