Surface heterogeneities, including roughness, significantly affect the adsorption, motion and interactions of particles at fluid interfaces. However, a systematic experimental study, linking surface roughness to particle wettability at a microscopic level, is currently missing. Here we synthesize a library of all-silica microparticles with uniform surface chemistry, but tuneable surface roughness and study their spontaneous adsorption at oil–water interfaces. We demonstrate that surface roughness strongly pins the particles' contact lines and arrests their adsorption in long-lived metastable positions, and we directly measure the roughness-induced interface deformations around isolated particles. Pinning imparts tremendous contact angle hysteresis, which can practically invert the particle wettability for sufficient roughness, irrespective of their chemical nature. As a unique consequence, the same rough particles stabilize both water-in-oil and oil-in-water emulsions depending on the phase they are initially dispersed in. These results both shed light on fundamental phenomena concerning particle adsorption at fluid interfaces and indicate future design rules for particle-based emulsifiers.

Janus particles are a unique class of multifunctional patchy particles combining two dissimilar chemical or physical functionalities at their opposite sides. The asymmetry characteristic for Janus particles allows them to self-assemble into sophisticated structures and materials not attainable by their homogeneous counterparts. Significant breakthroughs have recently been made in the synthesis of Janus particles and the understanding of their assembly. Nevertheless, the advancement of their applications is still a challenging field. In this Review, we highlight recent developments in the use of Janus particles as building blocks for functional materials. We provide a brief introduction into the synthetic strategies for the fabrication of JPs and their properties and assembly, outlining the existing challenges. The focus of this Review is placed on the applications of Janus particles for active interfaces and surfaces. Active functional interfaces are created owing to the stabilization efficiency of Janus particles combined with their capability for interface structuring and functionalizing. Moreover, Janus particles can be employed as building blocks to fabricate active functional surfaces with controlled chemical and topographical heterogeneity. Ultimately, we will provide implications for the rational design of multifunctional materials based on Janus particles.

A postsynthetic functionalization approach was used to tailor the hydrophobicity of DUT-67, a metal-organic framework (MOF) consisting of 8-connected Zr6O6(OH)2 clusters and 2,5-thiophenedicarboxylate as the ligand, using postsynthetic exchange of the modulator by fluorinated monocarboxylates. Water adsorption isotherms demonstrated that, by the incorporation of such hydrophobic molecules, the hydrophobicity of the inner surface of the network can be tuned. Furthermore, tolerance of the material toward the removal of adsorbed water can be significantly enhanced compared to the parent DUT-67 MOF.

We present the "on water" surface-initiated Cumediated controlled radical polymerization ("on water" SI-CuCRP) that converts hydrophobic monomers in aqueous reaction medium to polymer brushes at unparalleled speed and efficiency.The method allows the facile conversion of avariety of common monomers under most simple reaction conditions and with minimal monomer amounts to thicka nd homogeneous polymer brushes.The highly living character of the "on water" SI-CuCRP allowed the preparation of decablock (homo)polymer brushes and opens the pathway to sequentially controlled polymer brushes on solids.