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Title: DNA-mediated engineering of multicomponent enzyme crystals

Abstract

The ability to predictably control the coassembly of multiple nanoscale building blocks, especially those with disparate chemical and physical properties such as biomolecules and inorganic nanoparticles, has far-reaching implications in catalysis, sensing, and photonics, but a generalizable strategy for engineering specific contacts between these particles is an outstanding challenge. This is especially true in the case of proteins, where the types of possible interparticle interactions are numerous, diverse, and complex. In this paper, we explore the concept of trading protein–protein interactions for DNA–DNA interactions to direct the assembly of two nucleic-acid–functionalized proteins with distinct surface chemistries into six unique lattices composed of catalytically active proteins, or of a combination of proteins and DNA-modified gold nanoparticles. The programmable nature of DNA–DNA interactions used in this strategy allows us to control the lattice symmetries and unit cell constants, as well as the compositions and habit, of the resulting crystals. Finally, this study provides a potentially generalizable strategy for constructing a unique class of materials that take advantage of the diverse morphologies, surface chemistries, and functionalities of proteins for assembling functional crystalline materials.

Authors:
 [1];  [2];  [3]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. International Inst. for Nanotechnology
  2. Northwestern Univ., Evanston, IL (United States). International Inst. for Nanotechnology. Dept. of Materials Science and Engineering
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. International Inst. for Nanotechnology. Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE; USDOD; US Air Force Office of Scientific Research (AFOSR)
OSTI Identifier:
1182330
Grant/Contract Number:  
AC02-06CH11357; N00014-15-1-0043; FA9550-11-1-0275
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 112; Journal Issue: 15; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
ENGLISH
Subject:
59 BASIC BIOLOGICAL SCIENCES; nanoscience; biomaterials; self-assembly; superlattice; DNA-programmable assembly

Citation Formats

Brodin, Jeffrey D., Auyeung, Evelyn, and Mirkin, Chad A. DNA-mediated engineering of multicomponent enzyme crystals. United States: N. p., 2015. Web. doi:10.1073/pnas.1503533112.
Brodin, Jeffrey D., Auyeung, Evelyn, & Mirkin, Chad A. DNA-mediated engineering of multicomponent enzyme crystals. United States. https://doi.org/10.1073/pnas.1503533112
Brodin, Jeffrey D., Auyeung, Evelyn, and Mirkin, Chad A. 2015. "DNA-mediated engineering of multicomponent enzyme crystals". United States. https://doi.org/10.1073/pnas.1503533112. https://www.osti.gov/servlets/purl/1182330.
@article{osti_1182330,
title = {DNA-mediated engineering of multicomponent enzyme crystals},
author = {Brodin, Jeffrey D. and Auyeung, Evelyn and Mirkin, Chad A.},
abstractNote = {The ability to predictably control the coassembly of multiple nanoscale building blocks, especially those with disparate chemical and physical properties such as biomolecules and inorganic nanoparticles, has far-reaching implications in catalysis, sensing, and photonics, but a generalizable strategy for engineering specific contacts between these particles is an outstanding challenge. This is especially true in the case of proteins, where the types of possible interparticle interactions are numerous, diverse, and complex. In this paper, we explore the concept of trading protein–protein interactions for DNA–DNA interactions to direct the assembly of two nucleic-acid–functionalized proteins with distinct surface chemistries into six unique lattices composed of catalytically active proteins, or of a combination of proteins and DNA-modified gold nanoparticles. The programmable nature of DNA–DNA interactions used in this strategy allows us to control the lattice symmetries and unit cell constants, as well as the compositions and habit, of the resulting crystals. Finally, this study provides a potentially generalizable strategy for constructing a unique class of materials that take advantage of the diverse morphologies, surface chemistries, and functionalities of proteins for assembling functional crystalline materials.},
doi = {10.1073/pnas.1503533112},
url = {https://www.osti.gov/biblio/1182330}, journal = {Proceedings of the National Academy of Sciences of the United States of America},
issn = {0027-8424},
number = 15,
volume = 112,
place = {United States},
year = {Mon Mar 23 00:00:00 EDT 2015},
month = {Mon Mar 23 00:00:00 EDT 2015}
}

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Free Publicly Available Full Text
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Cited by: 111 works
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Works referenced in this record:

Nucleic Acid-Modified Nanostructures as Programmable Atom Equivalents: Forging a New “Table of Elements”*
book, August 2020


Maximizing DNA Loading on a Range of Gold Nanoparticle Sizes
journal, December 2006


Accurate design of co-assembling multi-component protein nanomaterials
journal, May 2014


Generation of protein lattices by fusing proteins with matching rotational symmetry
journal, July 2011


Nanohedra: Using symmetry to design self assembling protein cages, layers, crystals, and filaments
journal, February 2001


Design and self-assembly of two-dimensional DNA crystals
journal, August 1998


Enzyme cascades activated on topologically programmed DNA scaffolds
journal, March 2009


Computational Design of Self-Assembling Protein Nanomaterials with Atomic Level Accuracy
journal, May 2012


A comparison of successful and failed protein interface designs highlights the challenges of designing buried hydrogen bonds
text, January 2013


Life as a Nanoscale Phenomenon
journal, July 2008


A general strategy for the DNA-mediated self-assembly of functional nanoparticles into heterogeneous systems
journal, October 2013


DNA-guided crystallization of colloidal nanoparticles
journal, January 2008


Establishing the Design Rules for DNA-Mediated Programmable Colloidal Crystallization
journal, May 2010


An Overview of Structural DNA Nanotechnology
journal, July 2007


DNA-controlled assembly of a NaTl lattice structure from gold nanoparticles and protein nanoparticles
journal, October 2010


A general approach to DNA-programmable atom equivalents
journal, May 2013


Controlling the Lattice Parameters of Gold Nanoparticle FCC Crystals with Duplex DNA Linkers
journal, August 2008


Metal-directed, chemically tunable assembly of one-, two- and three-dimensional crystalline protein arrays
journal, March 2012


DNA-Mediated Assembly of Protein Heterodimers on Membrane Surfaces
journal, March 2013


From molecular to macroscopic via the rational design of a self-assembled 3D DNA crystal
journal, September 2009


Self-assembly and modular functionalization of three-dimensional crystals from oppositely charged proteins
journal, July 2014


Synthetically Programmable Nanoparticle Superlattices Using a Hollow Three-Dimensional Spacer Approach
book, March 2020


A DNA-based method for rationally assembling nanoparticles into macroscopic materials
journal, August 1996


Synthetically Programmable Nanoparticle Superlattices Using a Hollow Three-Dimensional Spacer Approach*
book, March 2020


Hierarchical Assembly of Plasmonic Nanostructures Using Virus Capsid Scaffolds on DNA Origami Templates
journal, July 2014


Protein Function in the Crystal
journal, June 1996


Functionalizing Designer DNA Crystals with a Triple-Helical Veneer
journal, March 2014


DNA-mediated nanoparticle crystallization into Wulff polyhedra
journal, November 2013


Synthetically programmable nanoparticle superlattices using a hollow three-dimensional spacer approach
journal, December 2011


Self-Assembly of Proteins into Designed Networks
journal, October 2003


DNA-Directed Three-Dimensional Protein Organization
journal, February 2012


Nanoparticle Superlattice Engineering with DNA
journal, October 2011


Self-Assembly of a Tetrahedral Lectin into Predesigned Diamondlike Protein Crystals
journal, August 1999


Nucleic Acid-Modified Nanostructures as Programmable Atom Equivalents: Forging a New “Table of Elements”
journal, May 2013


Protein crystalline frameworks with controllable interpenetration directed by dual supramolecular interactions
journal, August 2014


Transitioning DNA-Engineered Nanoparticle Superlattices from Solution to the Solid State
journal, July 2012


Functionalizing Designer DNA Crystals with a Triple-Helical Veneer
journal, March 2014


Supramolecular assembling systems formed by heme–heme pocket interactions in hemoproteins
journal, January 2012


Natural Nanochemical Building Blocks:  Icosahedral Virus Particles Organized by Attached Oligonucleotides
journal, August 2004


DNA-programmable nanoparticle crystallization
journal, January 2008


DNA-Directed Three-Dimensional Protein Organization
journal, February 2012


Phase Behavior of Nanoparticles Assembled by DNA Linkers
journal, January 2009


Nucleic Acid-Modified Nanostructures as Programmable Atom Equivalents: Forging a New “Table of Elements”*
book, March 2020


Electrostatic assembly of binary nanoparticle superlattices using protein cages
journal, December 2012


Programmable materials and the nature of the DNA bond
journal, February 2015


A Spectrophotometric Method for Measuring the Breakdown of Hydrogen Peroxide by Catalase
journal, March 1952


Reconstitution of Acid-denatured Catalase
journal, October 1963


Establishing the Design Rules for DNA-Mediated Programmable Colloidal Crystallization
journal, May 2010


Works referencing / citing this record:

Non-equilibrium anisotropic colloidal single crystal growth with DNA
journal, November 2018


Particle analogs of electrons in colloidal crystals
journal, June 2019


Self-Assembly of a 3D DNA Crystal Structure with Rationally Designed Six-Fold Symmetry
journal, August 2018


3D Lattice Engineering of Nanoparticles by DNA Shells
journal, February 2019


Transmutable nanoparticles with reconfigurable surface ligands
journal, February 2016


One-pot synthesis of oligonucleotide-grafted polymeric nanoparticles
journal, January 2020


Self-Assembly of a 3D DNA Crystal Structure with Rationally Designed Six-Fold Symmetry
journal, August 2018


Crystal engineering with DNA
journal, February 2019


DNA-Based Enzyme Reactors and Systems
journal, July 2016


Recent progress in live cell mRNA/microRNA imaging probes based on smart and versatile nanomaterials
journal, January 2018


Crystallizing protein assemblies via free and grafted linkers
journal, January 2019


Programmable DNA scaffolds for spatially-ordered protein assembly
journal, January 2016


Building expanded structures from tetrahedral DNA branching elements, RNA and TMV protein
journal, January 2018


Defining the Structure of a Protein–Spherical Nucleic Acid Conjugate and Its Counterionic Cloud
journal, March 2018


Self-Assembly of a Designed Nucleoprotein Architecture through Multimodal Interactions
journal, November 2018


Cross-Linked Micellar Spherical Nucleic Acids from Thermoresponsive Templates
journal, March 2017


General and Direct Method for Preparing Oligonucleotide-Functionalized Metal–Organic Framework Nanoparticles
journal, July 2017


Non-equilibrium anisotropic colloidal single crystal growth with DNA
journal, November 2018


Functional protein nanostructures: a chemical toolbox
journal, January 2018


DNA-Based Enzyme Reactors and Systems
journal, July 2016