Abstract

ConspectusDeveloping 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 develop a wider variety of functional DNA materials by the precise regulation of DNA assembly behaviors and topological structures. We further envision that our work on the design, synthesis, and applications of functional DNA materials is a typical paradigm for the “gene-like” precise construction of functional materials and hopefully will promote the development of materials genome.

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