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Self assembling nanoparticle enzyme clusters provide access to substrate channeling in multienzymatic cascades
by
Breger, Joyce C.
, Lasarte-Aragonés, Guillermo
, Klein, William P.
, Vranish, James N.
, Ellis, Gregory A.
, Thakur, Meghna
, Ancona, Mario G.
, Díaz, Sebastián A.
, Susumu, Kimihiro
, Hooe, Shelby L.
, Stewart, Michael H.
, Medintz, Igor L.
, Walper, Scott A.
, Oh, Eunkeu
in
631/45/603
/ 639/925/350/354
/ 82/83
/ 96/47
/ Biocatalysis
/ Catalysis
/ Channeling
/ Enzymes
/ Glycolysis
/ Humanities and Social Sciences
/ Kinetics
/ Mathematical models
/ multidisciplinary
/ Nanoclusters
/ Nanoparticles
/ Nanoparticles - chemistry
/ Quantum dots
/ Quantum Dots - chemistry
/ Saccharification
/ Science
/ Science (multidisciplinary)
/ Self-assembly
/ Stoichiometry
/ Structure-function relationships
/ Substrates
/ synthetic biology
2023
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Self assembling nanoparticle enzyme clusters provide access to substrate channeling in multienzymatic cascades
by
Breger, Joyce C.
, Lasarte-Aragonés, Guillermo
, Klein, William P.
, Vranish, James N.
, Ellis, Gregory A.
, Thakur, Meghna
, Ancona, Mario G.
, Díaz, Sebastián A.
, Susumu, Kimihiro
, Hooe, Shelby L.
, Stewart, Michael H.
, Medintz, Igor L.
, Walper, Scott A.
, Oh, Eunkeu
in
631/45/603
/ 639/925/350/354
/ 82/83
/ 96/47
/ Biocatalysis
/ Catalysis
/ Channeling
/ Enzymes
/ Glycolysis
/ Humanities and Social Sciences
/ Kinetics
/ Mathematical models
/ multidisciplinary
/ Nanoclusters
/ Nanoparticles
/ Nanoparticles - chemistry
/ Quantum dots
/ Quantum Dots - chemistry
/ Saccharification
/ Science
/ Science (multidisciplinary)
/ Self-assembly
/ Stoichiometry
/ Structure-function relationships
/ Substrates
/ synthetic biology
2023
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Self assembling nanoparticle enzyme clusters provide access to substrate channeling in multienzymatic cascades
by
Breger, Joyce C.
, Lasarte-Aragonés, Guillermo
, Klein, William P.
, Vranish, James N.
, Ellis, Gregory A.
, Thakur, Meghna
, Ancona, Mario G.
, Díaz, Sebastián A.
, Susumu, Kimihiro
, Hooe, Shelby L.
, Stewart, Michael H.
, Medintz, Igor L.
, Walper, Scott A.
, Oh, Eunkeu
in
631/45/603
/ 639/925/350/354
/ 82/83
/ 96/47
/ Biocatalysis
/ Catalysis
/ Channeling
/ Enzymes
/ Glycolysis
/ Humanities and Social Sciences
/ Kinetics
/ Mathematical models
/ multidisciplinary
/ Nanoclusters
/ Nanoparticles
/ Nanoparticles - chemistry
/ Quantum dots
/ Quantum Dots - chemistry
/ Saccharification
/ Science
/ Science (multidisciplinary)
/ Self-assembly
/ Stoichiometry
/ Structure-function relationships
/ Substrates
/ synthetic biology
2023
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Self assembling nanoparticle enzyme clusters provide access to substrate channeling in multienzymatic cascades
Journal Article
Self assembling nanoparticle enzyme clusters provide access to substrate channeling in multienzymatic cascades
2023
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Overview
Access to efficient enzymatic channeling is desired for improving all manner of designer biocatalysis. We demonstrate that enzymes constituting a multistep cascade can self-assemble with nanoparticle scaffolds into nanoclusters that access substrate channeling and improve catalytic flux by orders of magnitude. Utilizing saccharification and glycolytic enzymes with quantum dots (QDs) as a model system, nanoclustered-cascades incorporating from 4 to 10 enzymatic steps are prototyped. Along with confirming channeling using classical experiments, its efficiency is enhanced several fold more by optimizing enzymatic stoichiometry with numerical simulations, switching from spherical QDs to 2-D planar nanoplatelets, and by ordering the enzyme assembly. Detailed analyses characterize assembly formation and clarify structure-function properties. For extended cascades with unfavorable kinetics, channeled activity is maintained by splitting at a critical step, purifying end-product from the upstream sub-cascade, and feeding it as a concentrated substrate to the downstream sub-cascade. Generalized applicability is verified by extending to assemblies incorporating other hard and soft nanoparticles. Such self-assembled biocatalytic nanoclusters offer many benefits towards enabling minimalist cell-free synthetic biology.
Channeling between enzymes is a uniquely nanoscale phenomenon that can improve multienzymatic reaction rates. Here, the authors demonstrate that multistep enzyme cascades can self-assemble with nanoparticles into nanoclusters that access channeling and improve the underlying catalytic flux by several fold.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
Subject
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