Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Reversal of Catalytic Material Substrate Selectivity through Partitioning of Polymers in Hierarchically Ordered Virus-like Particle Frameworks

Journal Article · · Chemistry of Materials
Control over the selectivity of catalytic materials is a topic of growing interest. Virus-like particle (VLP) based materials such as protein macromolecular frameworks (PMFs) are promising for catalytic applications due to their ease of assembly, modular ability to encapsulate a variety of enzymes, and ease of separation from a reaction mixture. Here we demonstrate the reversal of the initially negative material charge through the titration of a positively charged polymer into the material, causing the reversal of guest molecule uptake and enzymatic activity of PMFs. The charge-inverse material partitions a charged enzyme substrate to concentrate the substrate near an enzyme incorporated within the material, generating up to 5.9-fold increases in enzyme activity toward the partitioned substrate over the excluded substrate. Here we also show that the polymer distributes heterogeneously through the material up to a point of saturation and the effects of guest macromolecules on the lattice parameters of PMFs.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
National Institutes of Health (NIH); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
2558072
Journal Information:
Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 21 Vol. 35; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (54)

RNA-Directed Packaging of Enzymes within Virus-like Particles journal November 2010
Genetically Programmed In Vivo Packaging of Protein Cargo and Its Controlled Release from Bacteriophage P22 journal June 2011
Enzyme Encapsulation by a Ferritin Cage journal October 2017
Optically Controlled Construction of Three‐Dimensional Protein Arrays journal May 2023
Molecular binding scaffolds increase local substrate concentration enhancing the enzymatic hydrolysis of VX nerve agent journal April 2020
Highly Selective Uptake and Release of Charged Molecules by pH‐Responsive Polydopamine Microcapsules journal June 2011
Clustered Nanocarriers: The Effect of Size on the Clustering of CCMV Virus-Like Particles With Soft Macromolecules: Clustered Nanocarriers: The Effect of Size on the Clustering … journal November 2014
Higher Order Assembly of Virus-like Particles (VLPs) Mediated by Multi-valent Protein Linkers journal January 2015
Protein cargo encapsulation by virus‐like particles: Strategies and applications journal November 2022
Production and applications of engineered viral capsids journal May 2014
Scaffolding protein regulates the polymerization of P22 coat subunits into icosahedral shells in vitro journal August 1988
Stepwise molecular display utilizing icosahedral and helical complexes of phage coat and decoration proteins in the development of robust nanoscale display vehicles journal August 2012
Use of the confined spaces of apo-ferritin and virus capsids as nanoreactors for catalytic reactions journal April 2015
Conformations of poly(allylamine hydrochloride) in electrolyte solutions: Experimental measurements and theoretical modeling journal February 2010
Encapsulation as a Strategy for the Design of Biological Compartmentalization journal February 2016
Diffusion and molecular partitioning in hierarchically complex virus-like particles journal March 2023
Polymer Coatings on Virus-like Particle Nanoreactors at Low Ionic Strength—Charge Reversal and Substrate Access journal April 2021
Cargo Retention inside P22 Virus-Like Particles journal August 2018
Protein Cages: From Fundamentals to Advanced Applications journal April 2022
Three-Dimensional Protein Cage Array Capable of Active Enzyme Capture and Artificial Chaperone Activity journal May 2019
Linker-Mediated Assembly of Virus-Like Particles into Ordered Arrays via Electrostatic Control journal April 2019
Substrate Partitioning into Protein Macromolecular Frameworks for Enhanced Catalytic Turnover journal September 2021
Multilayered Ordered Protein Arrays Self-Assembled from a Mixed Population of Virus-like Particles journal May 2022
Symmetry Controlled, Genetic Presentation of Bioactive Proteins on the P22 Virus-like Particle Using an External Decoration Protein journal August 2015
Modular Self-Assembly of Protein Cage Lattices for Multistep Catalysis journal November 2017
Templated Assembly of a Functional Ordered Protein Macromolecular Framework from P22 Virus-like Particles journal March 2018
Emerging Solutions for in Vivo Biocatalyst Immobilization: Tailor-Made Catalysts for Industrial Biocatalysis journal June 2021
Synthetic Virus-like Particles for Glutathione Biosynthesis journal November 2020
The Moderately Efficient Enzyme: Evolutionary and Physicochemical Trends Shaping Enzyme Parameters journal May 2011
Encapsulation of an Enzyme Cascade within the Bacteriophage P22 Virus-Like Particle journal November 2013
Assembling Enzymatic Cascade Pathways inside Virus-Based Nanocages Using Dual-Tasking Nucleic Acid Tags journal January 2017
Channeling by Proximity: The Catalytic Advantages of Active Site Colocalization Using Brownian Dynamics journal April 2010
High Capacity, Charge-Selective Protein Uptake by Polyelectrolyte Brushes journal April 2007
Nanoparticle-Templated Assembly of Viral Protein Cages journal April 2006
Nanoreactors by Programmed Enzyme Encapsulation Inside the Capsid of the Bacteriophage P22 journal May 2012
Biomimetic Antigenic Nanoparticles Elicit Controlled Protective Immune Response to Influenza journal April 2013
Self-assembling biomolecular catalysts for hydrogen production journal December 2015
A virus-based single-enzyme nanoreactor journal September 2007
Molecular exclusion limits for diffusion across a porous capsid journal May 2021
Nanoscale engineering of catalytic materials for sustainable technologies journal November 2020
Electrostatic self-assembly of virus–polymer complexes journal January 2011
Cargo–shell and cargo–cargo couplings govern the mechanics of artificially loaded virus-derived cages journal January 2016
Protein cage assembly across multiple length scales journal January 2018
Modular interior loading and exterior decoration of a virus-like particle journal January 2017
Tuning the catalytic properties of P22 nanoreactors through compositional control journal January 2020
Stabilizing viral nano-reactors for nerve-agent degradation journal January 2013
Virus factories: associations of cell organelles for viral replication and morphogenesis journal February 2005
Self-Assembly at All Scales journal March 2002
Viruses: Making Friends with Old Foes journal May 2006
Production and Characterization of a Thermostable Alcohol Dehydrogenase That Belongs to the Aldo-Keto Reductase Superfamily journal January 2006
Functions, Compositions, and Evolution of the Two Types of Carboxysomes: Polyhedral Microcompartments That Facilitate CO2 Fixation in Cyanobacteria and Some Proteobacteria journal September 2013
Regulation of Enzyme Function journal October 1969
Organizing Multi-Enzyme Systems into Programmable Materials for Biocatalysis journal March 2021
Bacteriophage P22 Capsid as a Pluripotent Nanotechnology Tool journal February 2023