Photocatalytic Regeneration of Nicotinamide Cofactors by Quantum Dot-Enzyme Biohybrid Complexes

被引:94
作者
Brown, Katherine A. [1 ]
Wilker, Molly B. [2 ]
Boehm, Marko [1 ]
Hamby, Hayden [2 ]
Dukovic, Gordana [2 ]
King, Paul W. [1 ]
机构
[1] Natl Renewable Energy Lab, Biosci Ctr, Golden, CO 80401 USA
[2] Univ Colorado, Dept Chem & Biochem, Campus Box 215, Boulder, CO 80309 USA
来源
ACS CATALYSIS | 2016年 / 6卷 / 04期
关键词
biohybrid; NADPH regeneration; photocatalysis; biocatalysis; quantum dots; BIOCATALYTIC REDOX REACTIONS; ELECTROCHEMICAL REGENERATION; VISIBLE-LIGHT; ELECTRON-TRANSFER; HYDROGENASE COMPLEXES; NADH; CDS; SEMICONDUCTOR; FERREDOXIN; REDUCTION;
D O I
10.1021/acscatal.5b02850
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We report the characterization of biohybrid complexes of CdSe quantum dots and ferredoxin NADP(-)(+)reductase for photocatalytic regeneration of NADPH. Illumination with visible light led to reduction of NADP+ to NADPH, with an apparent k(cat) of 1400 h(-1). Regeneration of NADPH was coupled to reduction of aldehydes to alcohols catalyzed by a NADPH-dependent alcohol dehydrogenase, Aldehyde with each NADPH molecule recycled an average of 7.5 times. The quantum yield both of NADPH and alcohol production were 5-6% for both products. Light-driven NADPH regeneration was also demonstrated in a multienzyme system, showing the capacity of QD-FNR complexes to drive continuous NADPH-dependent transformations.
引用
收藏
页码:2201 / 2204
页数:4
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  • [1] Direct electrochemical regeneration of the cofactor NADH on bare Ti, Ni, Co and Cd electrodes: The influence of electrode potential and electrode material
    Ali, Irshad
    Khan, Tariq
    Omanovic, Sasha
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2014, 387 : 86 - 91
  • [2] Direct electrochemical regeneration of the enzymatic cofactor 1,4-NADH employing nano-patterned glassy carbon/Pt and glassy carbon/Ni electrodes
    Ali, Irshad
    Gill, Amardeep
    Omanovic, Sasha
    [J]. CHEMICAL ENGINEERING JOURNAL, 2012, 188 : 173 - 180
  • [3] Photocatalytic Activity of Pt Nanoparticles for Visible Light-Driven Production of NADH
    Bhoware, Shrikant S.
    Kim, Ka Young
    Kim, Jin Ah
    Wu, Qiong
    Kim, Jinheung
    [J]. JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (05) : 2553 - 2557
  • [4] Diameter Dependent Electron Transfer Kinetics in Semiconductor-Enzyme Complexes
    Brown, Katherine A.
    Song, Qing
    Mulder, David W.
    King, Paul W.
    [J]. ACS NANO, 2014, 8 (10) : 10790 - 10798
  • [5] Characterization of Photochemical Processes for H2 Production by CdS Nanorod-[FeFe] Hydrogenase Complexes
    Brown, Katherine A.
    Wilker, Molly B.
    Boehm, Marko
    Dukovic, Gordana
    King, Paul W.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (12) : 5627 - 5636
  • [6] Controlled Assembly of Hydrogenase-CdTe Nanocrystal Hybrids for Solar Hydrogen Production
    Brown, Katherine A.
    Dayal, Smita
    Ai, Xin
    Rumbles, Garry
    King, Paul W.
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2010, 132 (28) : 9672 - 9680
  • [7] Light-Driven, Quantum Dot-Mediated Regeneration of FMN To Drive Reduction of Ketoisophorone by Old Yellow Enzyme
    Burai, Tarak Nath
    Panay, Aram Joel
    Zhu, Haiming
    Lian, Tianquan
    Lutz, Stefan
    [J]. ACS CATALYSIS, 2012, 2 (04): : 667 - 670
  • [8] Branched-chain keto acid decarboxylase from Lactococcus lactis (KdcA), a valuable thiamine diphosphate-dependent enzyme for asymmetric C-C bond formation
    Gocke, Doerte
    Nguyen, Cong Luan
    Pohl, Martina
    Stillger, Thomas
    Walter, Lydia
    Mueller, Michael
    [J]. ADVANCED SYNTHESIS & CATALYSIS, 2007, 349 (8-9) : 1425 - 1435
  • [9] Ferredoxin: NADP+ oxidoreductase as a target of Cd2+ inhibitory action - Biochemical studies
    Grzyb, Joanna
    Bojko, Monika
    Waloszek, Andrzej
    Strzalka, Kazimierz
    [J]. PHYTOCHEMISTRY, 2011, 72 (01) : 14 - 20
  • [10] Electrochemical regeneration of oxidoreductases for cell-free biocatalytic redox reactions
    Hollmann, F
    Schmid, A
    [J]. BIOCATALYSIS AND BIOTRANSFORMATION, 2004, 22 (02) : 63 - 88