Metal-binding peptides are versatile building blocks in supramolecular chemistry. We recently reported a class of crystalline materials formed through a combination of coiled-coil peptide self-association and metal coordination. Here, we probe the serendipitously discovered metal binding motif that drives the assembly and apply these insights to exert rational control over structure and morphology in the materials.
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A comparison of the collagen triple helix and coiled‐coil peptide building blocks on metal ion‐mediated supramolecular assembly
Metal ion‐mediated assembly of peptides is an intriguing method for developing novel biomaterials. In particular, peptide building blocks based on collagen triple helical and coiled‐coil peptides have been functionalized with metal‐binding ligands and assemble into hierarchical structures with diverse potential applications. This review outlines the use of metal‐mediated assembly with these supramolecular structures and highlights how changes in the building blocks lead to significant differences in structural morphologies, with the identity of the metal‐binding ligands and their placement on the building block as crucial aspects in the bottom‐up development of the assemblies.
more » « less- PAR ID:
- 10452899
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Peptide Science
- Volume:
- 113
- Issue:
- 2
- ISSN:
- 2475-8817
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Programmable self-assembly of smart, digital, and structurally complex materials from simple components at size scales from the macro to the nano remains a long-standing goal of material science. Here, we introduce a platform based on magnetic encoding of information to drive programmable self-assembly that works across length scales. Our building blocks consist of panels with different patterns of magnetic dipoles that are capable of specific binding. Because the ratios of the different panel-binding energies are scale-invariant, this approach can, in principle, be applied down to the nanometer scale. Using a centimeter-sized version of these panels, we demonstrate 3 canonical hallmarks of assembly: controlled polymerization of individual building blocks; assembly of 1-dimensional strands made of panels connected by elastic backbones into secondary structures; and hierarchical assembly of 2-dimensional nets into 3-dimensional objects. We envision that magnetic encoding of assembly instructions into primary structures of panels, strands, and nets will lead to the formation of secondary and even tertiary structures that transmit information, act as mechanical elements, or function as machines on scales ranging from the nano to the macro.more » « less
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Abstract The self-assembly of complex structures from a set of non-identical building blocks is a hallmark of soft matter and biological systems, including protein complexes, colloidal clusters, and DNA-based assemblies. Predicting the dependence of the equilibrium assembly yield on the concentrations and interaction energies of building blocks is highly challenging, owing to the difficulty of computing the entropic contributions to the free energy of the many structures that compete with the ground state configuration. While these calculations yield well known results for spherically symmetric building blocks, they do not hold when the building blocks have internal rotational degrees of freedom. Here we present an approach for solving this problem that works with arbitrary building blocks, including proteins with known structure and complex colloidal building blocks. Our algorithm combines classical statistical mechanics with recently developed computational tools for automatic differentiation. Automatic differentiation allows efficient evaluation of equilibrium averages over configurations that would otherwise be intractable. We demonstrate the validity of our framework by comparison to molecular dynamics simulations of simple examples, and apply it to calculate the yield curves for known protein complexes and for the assembly of colloidal shells.
