Nature produces exquisite material systems with hierarchical and dynamical structures over multiple length scales. For example, collagen, the most prevalent protein in the body, assembles into triple helices, fibrils, and fibers, providing structure to tissues in the body with transcendent properties. Inspired by such systems, we have designed hydrogel-based materials with molecular engineering principles to mimic key aspects of the structure, mechanical properties, and biochemical content of soft tissues. Specifically, we have synthesized assembling peptides that mimic the structure of collagen and decorated with reactive groups for incorporation within hydrogels formed by light-mediated thiol–ene click chemistry. The physical and chemical properties of the resulting matrix subsequently have been modulated by physical or covalent modification with fresh assembling or photoinitiated macromers integrated within the underlying network by applying heat or light, respectively. The initial and temporal multiscale properties of these systems have been probed with rheometry, electron microscopy, and super resolution microscopy, as well as indirectly with observations of cell response to these nanostructured synthetic extracellular matrices. This approach is promising for controlling the properties of well-defined hydrogels for a variety of applications, including disease modeling, regenerative medicine, and therapeutic delivery.

Utilizing assembling and orthogonal chemistries for the design of materials with multiscale property control

256th National Meeting (2018)

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