Nanostructures from Synthetic Genetic Polymers

Nanoscale objects of increasing complexity can be constructed from DNA or RNA. However, the scope of potential applications could be enhanced by expanding beyond the moderate chemical diversity of natural nucleic acids. Here, we explore the construction of nano‐objects made entirely from alternative building blocks: synthetic genetic polymers not found in nature, also called xeno nucleic acids (XNAs). Specifically, we describe assembly of 70 kDa tetrahedra elaborated in four different XNA chemistries (2′‐fluro‐2′‐deoxy‐ribofuranose nucleic acid (2′F‐RNA), 2′‐fluoroarabino nucleic acids (FANA), hexitol nucleic acids (HNA), and cyclohexene nucleic acids (CeNA)), as well as mixed designs, and a ∼600 kDa all‐FANA octahedron, visualised by electron microscopy. Our results extend the chemical scope for programmable nanostructure assembly, with implications for the design of nano‐objects and materials with an expanded range of structural and physicochemical properties, including enhanced biostability.

[1]  John C. Chaput,et al.  The structural diversity of artificial genetic polymers , 2015, Nucleic acids research.

[2]  C. Mao,et al.  A Case Study of the Likes and Dislikes of DNA and RNA in Self-Assembly. , 2015, Angewandte Chemie.

[3]  J. DeStefano,et al.  Selection of 2′-deoxy-2′-fluoroarabinonucleotide (FANA) aptamers that bind HIV-1 reverse transcriptase with picomolar affinity , 2015, Nucleic acids research.

[4]  Yamuna Krishnan,et al.  Designing DNA nanodevices for compatibility with the immune system of higher organisms. , 2015, Nature nanotechnology.

[5]  Thomas H. LaBean,et al.  Comparative Incorporation of PNA into DNA Nanostructures , 2015, Molecules.

[6]  Tim Liedl,et al.  One-Step Formation of "Chain-Armor"-Stabilized DNA Nanostructures. , 2015, Angewandte Chemie.

[7]  Antonio Manetto,et al.  Eintopfsynthese von “Kettenhemd”‐stabilisierten DNA‐Nanostrukturen , 2015 .

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

[9]  P. Fromme,et al.  Purification and assembly of thermostable Cy5 labeled γ-PNAs into a 3D DNA nanocage , 2014, Artificial DNA, PNA & XNA.

[10]  Vitor B. Pinheiro,et al.  Catalysts from synthetic genetic polymers , 2014, Nature.

[11]  P. Holliger,et al.  Towards applications of synthetic genetic polymers in diagnosis and therapy. , 2014, Current opinion in chemical biology.

[12]  Wade W Grabow,et al.  Multifunctional RNA Nanoparticles , 2014, Nano letters.

[13]  G. F. Joyce,et al.  The expanding view of RNA and DNA function. , 2014, Chemistry & biology.

[14]  William M. Shih,et al.  Addressing the Instability of DNA Nanostructures in Tissue Culture , 2014, ACS nano.

[15]  Pamela A. Silver,et al.  In vivo co-localization of enzymes on RNA scaffolds increases metabolic production in a geometrically dependent manner , 2014, Nucleic acids research.

[16]  Hao Yan,et al.  Structural DNA Nanotechnology: State of the Art and Future Perspective , 2014, Journal of the American Chemical Society.

[17]  Hao Yan,et al.  Multi-enzyme complexes on DNA scaffolds capable of substrate channelling with an artificial swinging arm. , 2014, Nature nanotechnology.

[18]  Luc Jaeger,et al.  RNA self-assembly and RNA nanotechnology. , 2014, Accounts of chemical research.

[19]  J. Piccirilli,et al.  Evidence for a group II intron-like catalytic triplex in the spliceosome , 2014, Nature Structural &Molecular Biology.

[20]  J. Steitz,et al.  The Noncoding RNA Revolution—Trashing Old Rules to Forge New Ones , 2014, Cell.

[21]  Almogit Abu-Horowitz,et al.  Universal computing by DNA origami robots in a living animal , 2014, Nature nanotechnology.

[22]  L. James Maher,et al.  Mechanical properties of DNA-like polymers , 2013, Nucleic acids research.

[23]  Jiye Shi,et al.  Scaffolded biosensors with designed DNA nanostructures , 2013 .

[24]  S. Howorka,et al.  Self-assembled DNA nanopores that span lipid bilayers. , 2013, Nano letters.

[25]  A. Serganov,et al.  A Decade of Riboswitches , 2013, Cell.

[26]  H. Sleiman,et al.  DNA nanostructure serum stability: greater than the sum of its parts. , 2013, Chemical communications.

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

[28]  T. G. Martin,et al.  Synthetic Lipid Membrane Channels Formed by Designed DNA Nanostructures , 2012, Science.

[29]  Akinori Kuzuya,et al.  Clear-cut observation of PNA invasion using nanomechanical DNA origami devices. , 2012, Chemical communications.

[30]  Björn Högberg,et al.  DNA origami delivery system for cancer therapy with tunable release properties. , 2012, ACS nano.

[31]  Carlos González,et al.  The solution structure of double helical arabino nucleic acids (ANA and 2′F-ANA): effect of arabinoses in duplex-hairpin interconversion , 2012, Nucleic acids research.

[32]  Vitor B. Pinheiro,et al.  A short adaptive path from DNA to RNA polymerases , 2012, Proceedings of the National Academy of Sciences.

[33]  D. Porath,et al.  Quasi 3D imaging of DNA–gold nanoparticle tetrahedral structures , 2012, Journal of physics. Condensed matter : an Institute of Physics journal.

[34]  John C. Chaput,et al.  Synthetic Genetic Polymers Capable of Heredity and Evolution , 2012, Science.

[35]  John C Chaput,et al.  Darwinian evolution of an alternative genetic system provides support for TNA as an RNA progenitor. , 2012, Nature chemistry.

[36]  Shawn M. Douglas,et al.  A Logic-Gated Nanorobot for Targeted Transport of Molecular Payloads , 2012, Science.

[37]  Hao Yan,et al.  Challenges and opportunities for structural DNA nanotechnology. , 2011, Nature nanotechnology.

[38]  Matthew J. A. Wood,et al.  DNA cage delivery to mammalian cells. , 2011, ACS nano.

[39]  Peixuan Guo,et al.  Fabrication of stable and RNase-resistant RNA nanoparticles active in gearing the nanomotors for viral DNA packaging. , 2011, ACS nano.

[40]  M. Manoharan,et al.  Unexpected origins of the enhanced pairing affinity of 2′-fluoro-modified RNA , 2010, Nucleic acids research.

[41]  H. Sleiman,et al.  Self-assembly of three-dimensional DNA nanostructures and potential biological applications. , 2010, Current opinion in chemical biology.

[42]  P. Herdewijn.  Nucleic Acids with a Six‐Membered ‘Carbohydrate’ Mimic in the Backbone , 2010, Chemistry & biodiversity.

[43]  Jung-Won Keum,et al.  Enhanced resistance of DNA nanostructures to enzymatic digestion. , 2009, Chemical communications.

[44]  Russell P. Goodman,et al.  High-resolution structural analysis of a DNA nanostructure by cryoEM. , 2009, Nano letters.

[45]  Andrew J Turberfield,et al.  Single-molecule protein encapsulation in a rigid DNA cage. , 2006, Angewandte Chemie.

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

[47]  H. Hansma,et al.  Building Programmable Jigsaw Puzzles with RNA , 2004, Science.

[48]  Andrew J Turberfield,et al.  The single-step synthesis of a DNA tetrahedron. , 2004, Chemical communications.

[49]  William M. Shih,et al.  A 1.7-kilobase single-stranded DNA that folds into a nanoscale octahedron , 2004, Nature.

[50]  C. Wilds,et al.  2'-Deoxy-2'-fluoro-beta-D-arabinonucleosides and oligonucleotides (2'F-ANA): synthesis and physicochemical studies. , 2000, Nucleic acids research.

[51]  T. Steitz,et al.  The structural basis of ribosome activity in peptide bond synthesis. , 2000, Science.

[52]  N. Seeman.  Nucleic acid junctions and lattices. , 1982, Journal of theoretical biology.