Unraveling and Manipulating of NADH Oxidation by Photogenerated Holes

Zhang, Shaohua; Shi, Jiafu; Chen, Yixuan; Huo, Qian; Li, Weiran; Wu, Yizhou; Sun, Yiying; Zhang, Yishan; Wang, Xiaodong; Jiang, Zhongyi

doi:10.1021/acscatal.0c00471

Cited by 50 publications

(38 citation statements)

References 47 publications

(93 reference statements)

Supporting

Mentioning

Contrasting

Unclassified

Order By: Relevance

“…Figure 1 shows a comparative study of photo‐, bio‐, and photobiocatalytic NADH oxidations. Photocatalytic oxidation of NADH was slow, regardless of catalysts, which is consistent with previous results [5b,18] . A putative mechanism of photocatalytic NADH oxidation was proposed (Scheme S1), based on previous work [25] .…”

Section: Methodssupporting

confidence: 90%

“…From the economic point of view, therefore, this photobiocatalytic NAD(P) + regeneration system may be applied for industrial catalytic oxidations. Furthermore, the high cofactor TTN suggests that the cofactors are highly stable in the photobiocatalytic process, in contrast to semiconductor photocatalysts that easily oxidize NAD(P)H into enzymatically inactive forms [5b] …”

Section: Methodsmentioning

confidence: 99%

See 1 more Smart Citation

Bioinspired Cooperative Photobiocatalytic Regeneration of Oxidized Nicotinamide Cofactors for Catalytic Oxidations

et al. 2021

View full text Add to dashboard Cite

Inspired by water‐forming NAD(P)H oxidases, a cooperative photobiocatalytic system has been designed to aerobically regenerate the oxidized nicotinamide cofactors. Photocatalysts enable NAD(P)H oxidation with O2 under visible‐light irradiation, producing H2O2 as a byproduct, which is subsequently used as an oxidant by the horseradish peroxidase mediator system (PMS) to oxidize NAD(P)H. The photobiocatalytic system shows a turnover frequency of 8800 min−1 in the oxidation of NAD(P)H. Photobiocatalytic NAD(P)H oxidation proceeds smoothly at pH 6–9. In addition to natural NAD(P)H, synthetic biomimetics are also good substrates for this regeneration system. Total turnover numbers of up to 180000 are obtained for the cofactor when the photobiocatalytic regeneration system is coupled with dehydrogenase‐catalyzed oxidations. It may be a promising protocol to recycle the oxidized cofactors for catalytic oxidations.

show abstract

Section: Methodssupporting

confidence: 90%

Section: Methodsmentioning

confidence: 99%

Bioinspired Cooperative Photobiocatalytic Regeneration of Oxidized Nicotinamide Cofactors for Catalytic Oxidations

et al. 2021

View full text Add to dashboard Cite

show abstract

“…We have identified by NMR spectroscopy and negative ion electrospray ionisation mass spectrometry nicotinamide, ADP-ribose, and its derivatives as the ultimate products generated. 11 The 1,4-NADH consumption rate (0.189 mM/h, Figure 2B) is equivalent to that of NAD + (0.185 mM/h, Figure 2A) under identical photocatalytic reaction conditions, suggesting 1,4-NADH will also be subject to fragmentation in a static-batch regeneration system.…”

Section: It Is Critical To Understand What Happens To the Nad + Reactant And Produced 14-nadh (If Any)mentioning

confidence: 90%

Improving Photocatalytic Energy Conversion via NAD(P)H

Jones

Burnett

Shi

et al. 2020

Joule

Self Cite

View full text Add to dashboard Cite

The reduced form of nicotinamide adenine dinucleotide (NAD(P)H) behaves as an energy/chemical "currency", carrying hydrogen in a biologically convertible form and donates electrons in numerous biotransformations and artificial photosynthesis. Its high cost necessitates its regeneration for reuse where photocatalysis using light energy is attractive. However, high NAD(P)H yield is only achievable via organic mediators to transfer electrons.Here, we analyse the current issues in catalytic NAD(P)H regeneration and show that a continuous-flow reactor system can realise selective NAD(P)H regeneration with 100% yield using Pt/C3N4 as a photocatalyst.

show abstract

“…Among them, the conversion of the human-made greenhouse gas CO 2 into valuable fuels/chemicals using solar energy is considered a promising and compelling approach to solar energy utilization because it aims to simultaneously solve problems regarding global energy and environment [ 114 ]. In particular, photoreaction coupled with enzymes provides a highly efficient, specific, and energy saving strategy for CO 2 conversion and has attracted special attention in recent years [ 115 ].…”

Section: Catalytic Reduction Of Comentioning

confidence: 99%

Research Progress in Conversion of CO2 to Valuable Fuels

Xiu

Liu

et al. 2020

Molecules

View full text Add to dashboard Cite

Rapid growth in the world’s economy depends on a significant increase in energy consumption. As is known, most of the present energy supply comes from coal, oil, and natural gas. The overreliance on fossil energy brings serious environmental problems in addition to the scarcity of energy. One of the most concerning environmental problems is the large contribution to global warming because of the massive discharge of CO2 in the burning of fossil fuels. Therefore, many efforts have been made to resolve such issues. Among them, the preparation of valuable fuels or chemicals from greenhouse gas (CO2) has attracted great attention because it has made a promising step toward simultaneously resolving the environment and energy problems. This article reviews the current progress in CO2 conversion via different strategies, including thermal catalysis, electrocatalysis, photocatalysis, and photoelectrocatalysis. Inspired by natural photosynthesis, light-capturing agents including macrocycles with conjugated structures similar to chlorophyll have attracted increasing attention. Using such macrocycles as photosensitizers, photocatalysis, photoelectrocatalysis, or coupling with enzymatic reactions were conducted to fulfill the conversion of CO2 with high efficiency and specificity. Recent progress in enzyme coupled to photocatalysis and enzyme coupled to photoelectrocatalysis were specially reviewed in this review. Additionally, the characteristics, advantages, and disadvantages of different conversion methods were also presented. We wish to provide certain constructive ideas for new investigators and deep insights into the research of CO2 conversion.

show abstract

Unraveling and Manipulating of NADH Oxidation by Photogenerated Holes

Cited by 50 publications

References 47 publications

Bioinspired Cooperative Photobiocatalytic Regeneration of Oxidized Nicotinamide Cofactors for Catalytic Oxidations

Bioinspired Cooperative Photobiocatalytic Regeneration of Oxidized Nicotinamide Cofactors for Catalytic Oxidations

Improving Photocatalytic Energy Conversion via NAD(P)H

Research Progress in Conversion of CO2 to Valuable Fuels

Contact Info

Product

Resources

About