21ENGBIO Controllable DNA polycatenanes of infinite length for intelligent biomaterials

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DNA is an ideal substrate from which to construct new materials for medical applications because it is sustainable, biodegradable, biocompatible, non-toxic, and highly programmable. DNA hydrogels have state-of-the-art applications in regenerative therapy (like stimulating new tissue growth from stem cells) and biologics delivery (like controlled, sustained release of insulin). They are squishy, gel-like materials made of water and web-like structures of DNA, and they can obtain unique properties when combined with nanomaterials. The disadvantages of current DNA hydrogels are in how their web-like structures of DNA are held together. Many rely on the ability of compatible DNA strands to stick together but this stickiness is susceptible changes in environmental conditions such as an increase in temperature which causes the structures to unravel. Adding small molecules to reinforce the DNA structures through cross-linking increases the manufacturing time and cost. Here, we will synthesise never-before-made DNA-based materials from polycatenanes. Polycatenanes are polymers in which molecular rings are mechanically linked together akin to the links of a chain. We have devised a strategy to make DNA polycatenanes of infinite and controllable lengths using enzymes to connect rings of DNA. In addition to enabling assembly 1D DNA chains, our strategy will enable construction of 2D and 3D DNA structures that require no cross-linking small molecules and will not unravel upon changes in environmental conditions. This work aims to seed development of a new family of structurally unique DNA-based biomaterials for programmable biologics delivery and patient-specific regenerative therapies.