DNA-Directed Assembly of Bienzymic Complexes from In Vivo Biotinylated NAD(P)H:FMN Oxidoreductase and Luciferase

Niemeyer, Christof M.; Koehler, Joerg; Wuerdemann, Chris

doi:10.1002/1439-7633(20020301)3:2/3<242::aid-cbic242>3.0.co;2-f

Cited by 188 publications

(156 citation statements)

References 8 publications

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“…They showed that the use of a simple DNA duplex could enhance the efficiency of many bienzymatic cascades, for example, NAD(P)H:FMN oxidoreductase and luciferase, 45 glucose oxidase (GOx) and horseradish peroxidase (HRP), 46 and two subdomains of cytochrome P450 BM3 in a cascade. 47 Because DNA duplexes can only regulate the distance between adjacent enzymes, high-order 2D and 3D DNA nanostructures can exert more precise control on multienzymatic cascades because of their abilities to regulate not only the distance but also other parameters, such as the arrangement and the concentration.…”

Section: Regulating Reaction Pathways For Bioinspired Nanofactoriesmentioning

confidence: 99%

Spatial regulation of synthetic and biological nanoparticles by DNA nanotechnology

Yang

Liu

2015

NPG Asia Mater

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Nanoparticles are among the most fascinating materials because of their unique size-dependent properties. The spatial positioning of the nanoparticles with a nanoscale precision will greatly enhance their potential for use in the fabrication of functional materials and devices. Recently, the development of DNA nanotechnology has enabled the construction of two-and three-dimensional, precisely addressable nanostructures and devices based on DNA sequence design and programmable assembly. Advances in conjugating DNA with nanoparticles can bridge these two technologies and provide scientists with a new tool to study material transportation and energy transfer at a nanometer scale. In this review, we summarize the recent progress in this emerging research field, which includes not only the static arrangements of inorganic nanoparticles but also the dynamic regulation of organic and biological units at a nanometer scale. With the rapid development in this field, new challenges and new possibilities will emerge and bring about fruitful achievements with a significant impact on future work.

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Section: Regulating Reaction Pathways For Bioinspired Nanofactoriesmentioning

confidence: 99%

Spatial regulation of synthetic and biological nanoparticles by DNA nanotechnology

Yang

Liu

2015

NPG Asia Mater

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“…27 Niemeyer et al reported multienzyme colocalization using DNA hybridization catalyzed cascaded reactions on planar surfaces, resulting in enhanced enzymatic activity. 20 Likewise, Muller and Niemeyer employed protein engineering combined with DNA-hybridization-directed evolution to develop supramolecular complexes using DNA as a scaffold for enzyme assembly. 21 They attached multiple enzymes by covalent binding to short single-stranded biotinylated and thiolated DNA oligonucleotides and brought them together using DNA-directed hybridization of short DNA with long complementary capture DNA to form a scaffold.…”

Section: ■ Introductionmentioning

confidence: 99%

Multienzyme Immobilization and Colocalization on Nanoparticles Enabled by DNA Hybridization

Feng

Mallapragada

Narasimhan

2015

Ind. Eng. Chem. Res.

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Multienzyme complexes (MECs) in nature exhibit highly efficient catalytic mechanisms in reaction cascades. Different strategies have been developed to colocalize enzymes on nanocarriers to improve multienzyme catalytic efficiency by mimicking MEC structure and function. Numerous studies have indicated that the spatial arrangement and orientation of multiple enzymes in confined spaces are critical in facilitating cooperative enzymatic activity in multienzyme colocalization. Biomolecule scaffolds based on DNA hybridization have attracted great attention because of their unique effective control of the relative positions of different enzymes in multienzyme colocalization. To demonstrate this concept, glucose oxidase (GOX) and horseradish peroxidase (HRP) were colocalized onto polystyrene nanoparticles via specific DNA hybridization. Colocalization of GOX and HRP was evidenced by Forster resonance energy transfer studies of the dyes labeling the two tag DNAs. Finally, it was observed that colocalization of GOX and HRP via DNA hybridization significantly improved both the overall reaction efficiency and the storage shelf life compared with those of the single enzyme immobilization mixture control. In summary, DNA-directed colocalization of multiple enzymes on nanoparticles is an effective way to control the relative positioning of enzymes to mimic MECs and enhance catalytic activity. ■ INTRODUCTIONEnzymes, which are nature's catalysts, are involved in many reactions that take place in living organisms and have evolved to catalyze various chemical reactions, including multistep reactions. 1−3 Multienzyme complexes (MECs) are composed of multiple enzyme subunits or large polypeptides with defined tertiary and quaternary structures containing compact multiple catalytic centers that are in close proximity to each other. 4,5 When enzymatic catalytic active sites are brought together, reaction intermediates can be transported rapidly among the active sites via a "substrate channeling" effect, which can reduce diffusion losses typically observed in free-enzyme catalytic processes, enabling the maintenance of high local concentrations of intermediates, which is especially critical for unstable intermediates. 6,7 In addition, MECs are known to significantly increase the overall reaction turnover efficiency. 8 These benefits of MECs have inspired researchers to design artificial MECs to mimic the structure and functionalities of MECs. A number of methodologies have been proposed to design artificial MECs, as reported in several recent studies and reviews. 9−15 In this context, enzyme-immobilization-based strategies exhibit great potential because of their economical reusability, enhanced kinetic performance, and higher stability under harsh operating conditions (e.g., extreme pH and temperature). 16,17 In particular, nanoparticles have attracted much attention because of their large surface areas for immobilization and no internal diffusion resistance, in contrast to porous materials. More specifically, polymeric nanoparticles ...

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“…This approach can be used, for instance, to generate multienzyme constructs as model systems for the investigation of "substratechanneling" processes. (12) On the other hand, the DNA-protein conjugates can be used to translate DNA arrays on surfaces into protein arrays (left part of Fig. 1).…”

Section: Introductionmentioning

confidence: 99%

Semisynthetic DNA-protein conjugates for fabrication of nucleic acid based nanostructures

Rabe¹,

Feldkamp²,

Niemeyer³

2008

AIP Conference Proceedings

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We here report on the developments of semisynthetic DNA-protein conjugates and their assembly into multi-component nanostructures. We describe the improvement of the DNA sequences embedded in such nanostructures by computational and analytical methods. Moreover, we report on the exploration of novel DNA conjugates of streptavidin or redox proteins with improved properties for the assembly of nucleic acid based nanostructures.

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DNA-Directed Assembly of Bienzymic Complexes from In Vivo Biotinylated NAD(P)H:FMN Oxidoreductase and Luciferase

Cited by 188 publications

References 8 publications

Spatial regulation of synthetic and biological nanoparticles by DNA nanotechnology

Spatial regulation of synthetic and biological nanoparticles by DNA nanotechnology

Multienzyme Immobilization and Colocalization on Nanoparticles Enabled by DNA Hybridization

Semisynthetic DNA-protein conjugates for fabrication of nucleic acid based nanostructures

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