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Self assembling nanoparticle enzyme clusters provide access to substrate channeling in multienzymatic cascades.
Breger, Joyce C; Vranish, James N; Oh, Eunkeu; Stewart, Michael H; Susumu, Kimihiro; Lasarte-Aragonés, Guillermo; Ellis, Gregory A; Walper, Scott A; Díaz, Sebastián A; Hooe, Shelby L; Klein, William P; Thakur, Meghna; Ancona, Mario G; Medintz, Igor L.
Afiliación
  • Breger JC; Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Vranish JN; Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Oh E; Department of Chemistry, Engineering, and Physics, Franciscan University of Steubenville, Steubenville, OH, 43952, USA.
  • Stewart MH; Optical Sciences Division, Code 5611, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Susumu K; Optical Sciences Division, Code 5611, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Lasarte-Aragonés G; Optical Sciences Division, Code 5611, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Ellis GA; Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Walper SA; College of Science, George Mason University, Fairfax, VA, 22030, USA.
  • Díaz SA; Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Hooe SL; Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Klein WP; Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Thakur M; Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
  • Ancona MG; National Research Council, Washington, D.C., 20001, USA.
  • Medintz IL; Center for Bio/Molecular Science and Engineering, Code 6900, U.S. Naval Research Laboratory, Washington, D.C., 20375, USA.
Nat Commun ; 14(1): 1757, 2023 03 30.
Article en En | MEDLINE | ID: mdl-36990995
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.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Puntos Cuánticos / Nanopartículas Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Reino Unido
Texto completo
Añadir a Mi BVS
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XML
PubMed Links
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Puntos Cuánticos / Nanopartículas Idioma: En Revista: Nat Commun Asunto de la revista: BIOLOGIA / CIENCIA Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Reino Unido