Self assembling nanoparticle enzyme clusters provide access to substrate channeling in multienzymatic cascades

Joyce C. Breger, James N. Vranish, Eunkeu Oh, Michael H. Stewart, Kimihiro Susumu, Guillermo Lasarte-Aragonés, Gregory A. Ellis, Scott A. Walper, Sebastián A. Díaz, Shelby L. Hooe, William P. Klein, Meghna Thakur, Mario G. Ancona and Igor L. Medintz ()
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Joyce C. Breger: U.S. Naval Research Laboratory
James N. Vranish: U.S. Naval Research Laboratory
Eunkeu Oh: U.S. Naval Research Laboratory
Michael H. Stewart: U.S. Naval Research Laboratory
Kimihiro Susumu: U.S. Naval Research Laboratory
Guillermo Lasarte-Aragonés: U.S. Naval Research Laboratory
Gregory A. Ellis: U.S. Naval Research Laboratory
Scott A. Walper: U.S. Naval Research Laboratory
Sebastián A. Díaz: U.S. Naval Research Laboratory
Shelby L. Hooe: U.S. Naval Research Laboratory
William P. Klein: U.S. Naval Research Laboratory
Meghna Thakur: U.S. Naval Research Laboratory
Mario G. Ancona: U.S. Naval Research Laboratory
Igor L. Medintz: U.S. Naval Research Laboratory

Nature Communications, 2023, vol. 14, issue 1, 1-20

Abstract: Abstract 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.

Date: 2023
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DOI: 10.1038/s41467-023-37255-9

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