Perforin-Mimicking Molecular Drillings Enable Macroporous Hollow Lignin Spheres for Performance-Configurable Materials.

Despite the first observations that the perforin can punch holes in target cells for live/dead cycles in the human immune system over 110 years ago, emulating this behaviour in materials science remains challenging. In this study, a perforin-mimicking molecular drilling strategy is employed to engineer macroporous hollow lignin spheres as performance-configurable catalysts, adhesives, and gels. Using a toolbox of over 20 molecular compounds, the local curvature of amphiphilic lignin is modulated to generate macroporous spheres with hole sizes ranging from 0-100 nm. Multiscale control is precisely achieved through non-covalent assembly directing catalysis, synthesis, and polymerization. Exceptional performance mutations correlated with the changes in hole size, including an increase in catalytic efficiency from 50% to 100%, transition from non-stick synthetics to ultrastrong adhesives (adhesion ∼18.3 MPa, exceeding that of classic epoxies), and transformation of viscous sols to tough nanogels. Thus, this study provides a robust and versatile non-covalent route for mimicking perforin-induced structural variations in cells, representing a significant stride towards the exquisite orchestration of assemblies over multiple length scales. This article is protected by copyright. All rights reserved.