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

被引：98

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

页码：2201 / 2204

页数：4

共 30 条

[1] Direct electrochemical regeneration of the cofactor NADH on bare Ti, Ni, Co and Cd electrodes: The influence of electrode potential and electrode material [J].

Ali, Irshad ;

Khan, Tariq ;

Omanovic, Sasha .

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 [J].

Ali, Irshad ;

Gill, Amardeep ;

Omanovic, Sasha .

CHEMICAL ENGINEERING JOURNAL, 2012, 188 :173-180

[3] Photocatalytic Activity of Pt Nanoparticles for Visible Light-Driven Production of NADH [J].

Bhoware, Shrikant S. ;

Kim, Ka Young ;

Kim, Jin Ah ;

Wu, Qiong ;

Kim, Jinheung .

JOURNAL OF PHYSICAL CHEMISTRY C, 2011, 115 (05) :2553-2557

[4] Diameter Dependent Electron Transfer Kinetics in Semiconductor-Enzyme Complexes [J].

Brown, Katherine A. ;

Song, Qing ;

Mulder, David W. ;

King, Paul W. .

ACS NANO, 2014, 8 (10) :10790-10798

[5] Characterization of Photochemical Processes for H2 Production by CdS Nanorod-[FeFe] Hydrogenase Complexes [J].

Brown, Katherine A. ;

Wilker, Molly B. ;

Boehm, Marko ;

Dukovic, Gordana ;

King, Paul W. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2012, 134 (12) :5627-5636

[6] Controlled Assembly of Hydrogenase-CdTe Nanocrystal Hybrids for Solar Hydrogen Production [J].

Brown, Katherine A. ;

Dayal, Smita ;

Ai, Xin ;

Rumbles, Garry ;

King, Paul W. .

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 [J].

Burai, Tarak Nath ;

Panay, Aram Joel ;

Zhu, Haiming ;

Lian, Tianquan ;

Lutz, Stefan .

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 [J].

Gocke, Doerte ;

Nguyen, Cong Luan ;

Pohl, Martina ;

Stillger, Thomas ;

Walter, Lydia ;

Mueller, Michael .

ADVANCED SYNTHESIS & CATALYSIS, 2007, 349 (8-9) :1425-1435

[9] Ferredoxin: NADP+ oxidoreductase as a target of Cd2+ inhibitory action - Biochemical studies [J].

Grzyb, Joanna ;

Bojko, Monika ;

Waloszek, Andrzej ;

Strzalka, Kazimierz .

PHYTOCHEMISTRY, 2011, 72 (01) :14-20

[10] Electrochemical regeneration of oxidoreductases for cell-free biocatalytic redox reactions [J].

Hollmann, F ;

Schmid, A .

BIOCATALYSIS AND BIOTRANSFORMATION, 2004, 22 (02) :63-88

← 1 2 3 →