Functional and Well‐Defined β‐Sheet‐Assembled Porous Spherical Shells by Surface‐Guided Peptide Formation

Abstract

Polypeptides have attracted widespread attention as building blocks for complex materials due to their ability to form higher‐ordered structures such as β‐sheets. However, the ability to precisely control the formation of well‐defined β‐sheet‐assembled materials remains challenging as β‐sheet formation tends to lead to ill‐defined and unprocessable aggregates. This work reports a simple, rapid, and robust strategy to form well‐defined peptide β‐sheet‐assembled shells (i.e., hollow spheres) by employing surface‐initiated N‐carboxyanhydride ring‐opening polymerization under a highly efficient surface‐driven approach. The concept is demonstrated by the preparation of enzyme‐degradable rigid shell architectures composed of H‐bonded poly(L‐valine) (PVal) grafts with porous and sponge‐like surface morphology. The porous PVal‐shells exhibit a remarkable and unprecedented ability to non‐covalently entrap metal nanoparticles, proteins, drug molecules, and biorelevant polymers, which could potentially lead to a diverse range of biodegradable and functional platforms for applications ranging from therapeutic delivery to organic catalysis.

Spider-silk inspired polymeric networks by harnessing the mechanical potential of β-sheets through network guided assembly

“…olypeptides are the fundamental building blocks of many naturally occurring materials due to their ability to fold into specific yet complex molecular architectures, including αhelices and β-sheets [1][2][3][4] . The ability to form these secondary structures in response to various environmental cues (e.g.…”

“…7) shows that with more intense β-sheet conformations, the networks (both hydrogels and cryogels) are more thermally stable, as characterised by higher remaining fraction between 200 and 300°C. Opposing energetic effects of enthalpically driven hydrogen bonding of β-sheets and entropically driven hydrophobic interactions of the isopropyl side-chain of Val residues are believed to contribute to such superb resistance to elevated thermal treatment 4,56 . All the networks have an onset temperature of mass loss between 150 and 200°C, corresponding to the disintegration of initial networks.…”

Architectural Design of Self‐Assembled Hollow Superstructures

“…It is noteworthy that assembled hollow superstructures have been confirmed to be among the most useful materials in biomedicine, particularly with regard to disease diagnosis and therapy . Their high level of applicability is due to their distinct advantages, including in high‐sensitivity imaging and by providing cavities that offer greater drug‐loading capacity.…”

Palladium Supported Porous Polyurea Frameworks as an Efficient Heterogeneous Catalyst for Suzuki-Miyaura Cross-coupling Reaction

“…1 Porous organic polymers (POPs) are noticeable materials with special properties such as surface permanent porosity and a large surface area. In addition, POPs have been recently used in gas storage, 2-10 sensing, 11,12 light emitting, 4,11,[13][14][15] and heterogeneous catalysts [16][17][18][19][20] because of their ability to control pore size and tune functional groups by easy chemical reactions. Especially in recent years, significantly advances have been made to use POPs as heterogeneous phase catalysts because many reactions use expensive noble metals as catalysts.…”