Structurally Ordered Nanowire Formation from Co-Assembly of DNA Origami and Collagen-Mimetic Peptides.

We describe the co-assembly of two different building units: collagen-mimetic peptides and DNA origami. Two peptides CP++ and sCP++ are designed with a sequence comprising a central block (Pro-Hyp-Gly) and two positively charged domains (Pro-Arg-Gly) at both N- and C-termini. Co-assembly of peptides and DNA origami two-layer (TL) nanosheets affords the formation of one-dimensional nanowires with repeating periodicity of ∼10 nm. Structural analyses suggest a face-to-face stacking of DNA nanosheets with peptides aligned perpendicularly to the sheet surfaces. We demonstrate the potential of selective peptide-DNA association between face-to-face and edge-to-edge packing by tailoring the size of DNA nanostructures. This study presents an attractive strategy to create hybrid biomolecular assemblies from peptide- and DNA-based building blocks that takes advantage of the intrinsic chemical and physical properties of the respective components to encode structural and, potentially, functional complexity within readily accessible biomimetic materials.

[1]  J. Reif,et al.  DNA-Templated Self-Assembly of Protein Arrays and Highly Conductive Nanowires , 2003, Science.

[2]  P. Rothemund.  Folding DNA to create nanoscale shapes and patterns , 2006, Nature.

[3]  W. Chiu,et al.  Designer nanoscale DNA assemblies programmed from the top down , 2016, Science.

[4]  S. Stupp,et al.  Precision templating with DNA of a virus-like particle with peptide nanostructures. , 2013, Journal of the American Chemical Society.

[5]  R. Raines,et al.  Peptide tessellation yields micron-scale collagen triple helices , 2016, Nature chemistry.

[6]  J. Fallas,et al.  Multi-hierarchical self-assembly of a collagen mimetic peptide from triple helix to nanofibre and hydrogel. , 2011, Nature chemistry.

[7]  K. Okuyama,et al.  Chain Dimensions and Hydration Behavior of Collagen Model Peptides in Aqueous Solution: [Glycyl-4(R)-hydroxyprolyl-4(R)-hydroxyproline]n, [Glycylprolyl-4(R)-hydroxyproline]n, and Some Related Model Peptides , 2008 .

[8]  M. Ryadnov,et al.  A De Novo Virus-Like Topology for Synthetic Virions. , 2016, Journal of the American Chemical Society.

[9]  Rong Ni,et al.  Tuning the Inter-nanofibril Interaction To Regulate the Morphology and Function of Peptide/DNA Co-assembled Viral Mimics. , 2017, Angewandte Chemie.

[10]  N. Seeman,et al.  Design and self-assembly of two-dimensional DNA crystals , 1998, Nature.

[11]  Chin-Lin Guo,et al.  Computational design of co-assembling protein–DNA nanowires , 2015, Nature.

[12]  Paramjit S. Arora,et al.  Amyloid fibrils nucleated and organized by DNA origami constructions , 2014, Nature nanotechnology.

[13]  R. Mann,et al.  The role of DNA shape in protein-DNA recognition , 2009, Nature.

[14]  Y. Lim,et al.  Reciprocal Self-Assembly of Peptide-DNA Conjugates into a Programmable Sub-10-nm Supramolecular Deoxyribonucleoprotein. , 2016, Angewandte Chemie.

[15]  R. Nolte,et al.  Encapsulation of DNA-templated chromophore assemblies within virus protein nanotubes. , 2010, Angewandte Chemie.

[16]  Roland Brock,et al.  Design and self-assembly of simple coat proteins for artificial viruses. , 2014, Nature nanotechnology.

[17]  K. Holmes,et al.  Structure of RNA and RNA binding site in tobacco mosaic virus from 4-Å map calculated from X-ray fibre diagrams , 1977, Nature.

[18]  N. Seeman,et al.  Programmable materials and the nature of the DNA bond , 2015, Science.

[19]  K. Salaita,et al.  Structurally defined nanoscale sheets from self-assembly of collagen-mimetic peptides. , 2014, Journal of the American Chemical Society.

[20]  Vikas Nanda,et al.  Dissecting Electrostatic Contributions to Folding and Self-Assembly Using Designed Multicomponent Peptide Systems. , 2016, Journal of the American Chemical Society.

[21]  Luvena L. Ong,et al.  Three-Dimensional Structures Self-Assembled from DNA Bricks , 2012, Science.

[22]  Chunfu Xu,et al.  Structurally homogeneous nanosheets from self-assembly of a collagen-mimetic peptide. , 2014, Angewandte Chemie.

[23]  Hendrik Dietz,et al.  Self-assembly of genetically encoded DNA-protein hybrid nanoscale shapes , 2017, Science.

[24]  B. Cullity,et al.  Elements of X-ray diffraction , 1957 .

[25]  Keita Miyama,et al.  Crystal structure of (Gly-Pro-Hyp)(9) : implications for the collagen molecular model. , 2012, Biopolymers.

[26]  Andrew R Thomson,et al.  De novo protein design: how do we expand into the universe of possible protein structures? , 2015, Current opinion in structural biology.

[27]  Charles M. Rubert Pérez,et al.  Tuning the thermosensitive properties of hybrid collagen peptide-polymer hydrogels. , 2014, Chemical communications.

[28]  C R Cantor,et al.  Oligonucleotide-directed self-assembly of proteins: semisynthetic DNA--streptavidin hybrid molecules as connectors for the generation of macroscopic arrays and the construction of supramolecular bioconjugates. , 1994, Nucleic acids research.

[29]  Paul C. Wang,et al.  Virus-Inspired Self-Assembled Nanofibers with Aggregation-Induced Emission for Highly Efficient and Visible Gene Delivery. , 2017, ACS applied materials & interfaces.

[30]  J. Ramshaw,et al.  Prediction of Collagen Stability from Amino Acid Sequence* , 2005, Journal of Biological Chemistry.

[31]  Zhigang Jiang,et al.  Rational Design of Multilayer Collagen Nanosheets with Compositional and Structural Control. , 2015, Journal of the American Chemical Society.