Gene-like Precise Construction of Functional DNA Materials

Abstract

Conspectus Developing a new system of material chemistry is an important molecular foundation for the design and preparation of functional materials, which resembles the preparation of raw materials such as bricks for constructing a building that determines the quality of the building. However, precisely controlling the synthesis processes and structures of functional materials always remains a grand challenge. It is expected to propose a paradigm of “gene-like” precise construction to realize the rational synthesis of functional materials, i.e., a “structure-function-application” principle for the precise construction. As the core genetic material of life, the DNA molecule is a bioactive macromolecule that can accurately encode genetic information and also can act as the generic molecular building block for the precise construction of functional materials. In this Account, we describe our work on the design and construction of functional DNA materials, to illustrate the principle of “gene-like” construction of functional DNA materials. The DNA molecule shows the unique advantages in the “gene-like” construction of functional materials, mainly including the precise arrangement of bases (monomers), the controllable design and assembly of structure, the precise transmission of sequence information, and customization of function. First, the number and sequence of four deoxynucleotide monomers that constitute the DNA strand can be rationally designed and accurately synthesized. Second, the sequence information on DNA endows the precise and efficient assembly of DNA molecules and ensures the precise regulation on the specific biological functions of functional DNA materials. Third, the functions of DNA materials can couple with the biological environments, so as to achieve the predetermined applications. Based on the scale of the constructed DNA materials, we categorize DNA materials into three classes: molecular scale, nanoscale, and macroscale. At the molecular scale, the representative material is branched DNA-based materials; the construction strategies mainly include target-triggered polymerization, enzymatic extension, and hybrid coupling; the applications mainly include the nonenzymatic detection of base mutation, the construction of artificial cells for the study of compartmentalization and the confinement effect, and the regulation of optical and antibacterial properties of supernanoclusters. At the nanoscale, the representative material is the DNA nanocomplex; the construction strategies mainly include hybridization with polymer, small molecule, and metal ions; the applications mainly include gene drug delivery and luminescence bioimaging. At the macroscale, the representative material is the DNA hydrogel; the construction strategies mainly include double-rolling circle amplification (double-RCA), multistage-RCA, and chemical cross-linking; the applications mainly include cell isolation, cell delivery, antibacterial agents, and self-healing electric circuits. Based on the “gene-like” paradigm, we expect to d...

DNA Supramolecular Assembly on Micro/Nanointerfaces for Bioanalysis

“…10−12 Moreover, with this programmable molecule, customized functional modules can be rationally designed. 13 For examples, DNA aptamers exhibit specific recognition on target molecules; 14 responsive sequences such as DNA i-motifs and G-duplexes show conformational transformation upon stimuli; 15 catalytic DNAzymes initiate cleavage toward target sequences. 16,17 Because of these unique properties and functions, DNA has been extensively applied in the field of bioanalysis, including bioseparation, 18 biosensing, 19 biological detection, 20 and imaging.…”

“…Recently, DNA has been a rising programmable biomaterial for building multifunctional systems. , From the perspective of materials chemistry, DNA can be accurately synthesized from four deoxynucleotide monomers, including adenine (A), guanine (G), cytosine (C), and thymine (T). On the other hand, the unique intermolecular hydrogen bonding between A and T, C and G ensures accurate base pairing between complementary single-strand DNA chains, and thus the structure of DNA can be accurately manipulated on the molecular scale. − Moreover, with this programmable molecule, customized functional modules can be rationally designed . For examples, DNA aptamers exhibit specific recognition on target molecules; responsive sequences such as DNA i-motifs and G-duplexes show conformational transformation upon stimuli; catalytic DNAzymes initiate cleavage toward target sequences. , Because of these unique properties and functions, DNA has been extensively applied in the field of bioanalysis, including bioseparation, biosensing, biological detection, and imaging …”

Dynamic assembly of DNA-ceria nanocomplex in living cells generates artificial peroxisome

“…Recently, we developed a DNA-based pH-responsive dynamic system that successfully achieved topological transformation from nanoparticles to organelle-like hydrogel architectures specifically mediated by lysosomal acidic condition inside living cells 27 . Moreover, DNA molecule can be easily hybridized with additional components to introduce more functional modules, such as ceria as redox enzyme mimetics, enabling DNA-based materials with organelle-like activities 28 .…”

Construction of rolling circle amplification-based DNA nanostructures for biomedical applications

“…The number and sequence of four nucleotide subunits can be accurately synthesized by rational design, which endows a DNA molecule with excellent structural accuracy. 4,5 By virtue of sequence programmability, structural predictability, and function controllability, DNA has emerged as a promising building block to fabricate functional nanomaterials. [6][7][8][9][10] Rolling circle amplification (RCA) is an isothermal enzymatic reaction in which the polymerase synthesizes the highly tandem repeating sequences from a circular DNA template.…”

“…The number and sequence of four nucleotide subunits can be accurately synthesized by rational design, which endows a DNA molecule with excellent structural accuracy. 4,5 By virtue of sequence programmability, structural predictability, and function controllability, DNA has emerged as a promising building block to fabricate functional nanomaterials. 6–10…”