Joyce C. Breger, Drew Lysne, Kimihiro Susumu, Michael H. Stewart, Eunkeu Oh, Gregory A. Ellis, Igor L. Medintz
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引用次数: 0
Abstract
Allowing coupled enzymes to crosslink with nanoparticles (NPs) into nanoclusters has been shown to facilitate them engaging in the most efficient form of multienzymatic catalysis, namely that of intermediary channeling. Utilizing a previously validated nanoparticle-scaffolded seven enzyme cascade from glycolysis that processes glucose into 3-phosphoglycerate, we begin by confirming that non-cadmium containing ZnSe/ZnS core/shell quantum dots (QDs) made from non-toxic and earth abundant materials can replace Cd-containing QDs as a scaffolding material in the multienzyme clusters while still providing access to improved channeling activity. We then investigate the role of enzyme assembly order within mixed NP systems that consist of both spherical QDs and rectangular 2-dimensional nanoplatelets (NPLs). Along with physicochemical confirmation of enzyme assembly to the QDs and enzyme-induced cluster formation, the rate of overall catalytic flux for each of the systems was monitored under different assembly conditions. The results reveal that adjusting relative NP concentration normalized to surface area, enzyme assembly order, and choice of initial material in any mixed NP clustered configuration are critical to attaining further improvements in catalytic flux via channeling. The potential ramifications of these observations in the context of assembling designer biosynthetic cascades that use bulk feedstock materials derived from agriculture to create new and useful products are then discussed.
Graphical Abstract
Schematic of a self-assembled mixed QD-NPL-enzyme system engaged in 7-enzyme sequential substrate channeling.
期刊介绍：
The objective of the Journal of Nanoparticle Research is to disseminate knowledge of the physical, chemical and biological phenomena and processes in structures that have at least one lengthscale ranging from molecular to approximately 100 nm (or submicron in some situations), and exhibit improved and novel properties that are a direct result of their small size.
Nanoparticle research is a key component of nanoscience, nanoengineering and nanotechnology.
The focus of the Journal is on the specific concepts, properties, phenomena, and processes related to particles, tubes, layers, macromolecules, clusters and other finite structures of the nanoscale size range. Synthesis, assembly, transport, reactivity, and stability of such structures are considered. Development of in-situ and ex-situ instrumentation for characterization of nanoparticles and their interfaces should be based on new principles for probing properties and phenomena not well understood at the nanometer scale. Modeling and simulation may include atom-based quantum mechanics; molecular dynamics; single-particle, multi-body and continuum based models; fractals; other methods suitable for modeling particle synthesis, assembling and interaction processes. Realization and application of systems, structures and devices with novel functions obtained via precursor nanoparticles is emphasized. Approaches may include gas-, liquid-, solid-, and vacuum-based processes, size reduction, chemical- and bio-self assembly. Contributions include utilization of nanoparticle systems for enhancing a phenomenon or process and particle assembling into hierarchical structures, as well as formulation and the administration of drugs. Synergistic approaches originating from different disciplines and technologies, and interaction between the research providers and users in this field, are encouraged.
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