Superomniphobic surfaces display contact angles >150° and low contact angle hysteresis with essentially all contacting liquids. In this work, we report surfaces that display superomniphobicity with a range of different non-Newtonian liquids, in addition to superomniphobicity with a wide range of Newtonian liquids. Our surfaces possess hierarchical scales of re-entrant texture that significantly reduce the solid-liquid contact area. Virtually all liquids including concentrated organic and inorganic acids, bases, and solvents, as well as viscoelastic polymer solutions, can easily roll off and bounce on our surfaces. Consequently, they serve as effective chemical shields against virtually all liquids--organic or inorganic, polar or nonpolar, Newtonian or non-Newtonian.

Phenolic materials have long been known for their use in inks, wood coatings, and leather tanning. However, recently there has been a renewed interest in engineering advanced materials from phenolic building blocks. The intrinsic properties of phenolic compounds, such as metal chelation, hydrogen bonding, pH responsiveness, redox potentials, radical scavenging, polymerization, and light absorbance, have made them a distinct class of structural motifs for the synthesis of functional materials. Materials prepared from phenolic compounds often retain many of these useful properties with synergistic effects in applications ranging from catalysis to biomedicine. The present review provides an overview of the diverse functional materials that can be prepared from phenolic building blocks, bridging the various fields currently studying and using phenolic compounds. Natural and synthetic phenolic compounds are first discussed, followed by the assembly of functional materials. The engineered phenolic materials are grouped under three broad categories: thin films (e.g., metal-phenolic networks and polydopamine); particles (e.g., metal-organic frameworks and superstructures); and bulk materials (e.g., gels). Applications of phenolic-based materials are then presented, focusing mainly on mechanical (e.g., adhesives), biological (e.g., drug delivery), and environmental and energy (e.g., separation and catalysis) applications. Several examples of their emerging applications are also included. Finally, potential routes for the continued integration of disparate fields using phenolic building blocks and fundamental questions still requiring investigation are highlighted, and an outlook of the field is provided.

High-performing coatings that durably and fully repel liquids are of interest for fundamental research and practical applications. Such coatings should allow for droplet beading, roll off and bouncing, which is difficult to achieve for ultralow surface tension liquids. Here, we report a bottom-up approach for preparing superrepellent coatings using a mixture of fluoro-silanes and cyanoacrylate. Upon application onto surfaces, the coatings assemble into thin films of locally multi-reentrant hierarchical structures with very low surface energy. The resulting material is superrepellent to solvents, acids and bases, polymer solutions and ultralow surface tension liquids, characterized by ultrahigh surface contact angles (>150°) and negligible roll-off angles (~0°). Furthermore, the coatings are transparent, durable and demonstrate universal liquid bouncing, tailored responsiveness and anti-freezing properties, being thus a promising alternative to existing artificial superrepellent coatings.3 Repellent coatings are of broad interest for investigating fundamental interfacial phenomena 1-4 , as well as for practical applications in areas such as self-cleaning 5-7 , chemical shielding 8 , heat transfer 3 , wet adhesives 9 , drag-reduction 10 , anti-fouling 11 , separations and membranes 12,13 , fogharvesting 14 , self-assembly 15 , and icephobicity and anti-freezing 2,16,17 . Combining sophisticated microstructures possessing reentrant 18 or double-reentrant textures 19 with low surface energy chemical modifications 20-22 result in state-of-the-art techniques for the preparation of repellent surfaces (i.e. surfaces with apparent contact angles θ * > 150°, which are considered superhydrophobic or superoleophobic for water and oil, respectively). However, engineering high-performing surfaces that are superrepellent (i.e. droplet roll-off angles ~0°) even to liquids with ultralow surface tensions (i.e. <20 mN m -1 ; e.g., n-hexane and n-pentane) remains challenging because of their low solid-liquid interfacial energy (see Supplementary Figs. 1 and 2 for detailed discussion). To date, this has only been possible using a "top-down", multi-step etching-based approach 19 , which can have limited applicability and versatility due to a lack of robustness, e.g., break-in of liquid. StrategyThe overall performance of a coating is governed by a range of properties 23 -including surface morphology, binding forces, surface chemistry, and other physical and mechanical characteristics-whereas surface repellence to liquids is primarily dependent on the surface texture and chemistry 20,24 . As these factors are interrelated, the design of simple and versatile superrepellent coatings is difficult. For example, increasing surface roughness may be used to minimize the liquid-solid contact area, which favours ultrahigh contact angles and ultralow rolloff angles. However, increased surface roughness can also compromise the transparency and durability of a coating 20,25 . Additionally, the responsiveness of a coating may enable surfaces

The self-assembly of molecular building blocks into well-defined macroscopic materials is desirable for developing emergent functional materials. However, the selfassembly of molecules into macroscopic materials remains challenging, in part because of limitations in controlling the growth and robustness of the materials. Herein, we report the molecular self-assembly of nano-to macroscopic free-standing materials through the coordination of metals with natural phenolic molecules. Our method involves a simple and scalable solution-based template dipping process in precomplexed metal−phenolic solutions, enabling the fabrication of free-standing macroscopic materials of customized architectures (2D and 3D geometries), thickness (about 10 nm to 5 μm), and chemical composition (different metals and phenolic ligands). Our macroscopic free-standing materials can be physically folded and unfolded like origami, yet are selectively degradable. Furthermore, metal nanoparticles can be grown in the macroscopic free-standing films, indicating their potential for future applications in biotechnology and catalysis.

Mesoporous metal-organic networks have attracted widespread interest owing to their potential applications in diverse fields including gas storage, separations, catalysis, and drug delivery. Despite recent advances, the synthesis of metal-organic networks with large and ordered mesochannels (>20 nm), which are important for loading, separating, and releasing macromolecules, remains a challenge. Herein, we report a templating strategy using sacrificial double cubic network polymer cubosomes ( 3 ) to synthesize ordered mesoporous metal-phenolic particles (meso-MPN particles) with a large pore (~40 nm) single cubic network ( 3 ). We demonstrate that the large pore network and the phenolic groups in the meso-MPN particles enable high loadings of various proteins (e.g., horseradish peroxidase (HRP), bovine hemoglobin, immunoglobulin G, and glucose oxidase (GOx)), which have different shapes, charges, and sizes (i.e., molecular weights spanning 44-160 kDa). For example, GOx loading in the meso-MPN particles was 362 mg g −1 , which is ~6-fold higher than the amount loaded in commercially available SiO2 particles with an average pore size of 50 nm. Furthermore, we show that HRP, when loaded in the meso-MPN particles (486 mg g −1 ), retained ~82% activity of free HRP in solution and can be recycled at least 5 times with a minimal (~13%) decrease in HRP activity, which exceeds HRP performance in 50-nm pore SiO2 particles (~36% retained activity and ~30% activity loss when recycled 5 times). Considering the wide selection of naturally abundant polyphenols (>8000 species) and metal ions available, the present cubosome-enabled strategy is expected to provide new avenues for designing a range of meso-MPN particles for various applications.

We report a facile strategy for engineering diverse particles based on the supramolecular assembly of natural polyphenols and a self-polymerizable aromatic dithiol. In aqueous conditions, uniform and size-tunable supramolecular particles are assembled through π–π interactions as mediated by polyphenols. Owing to the high binding affinity of phenolic motifs present at the surface, these particles allow for the subsequent deposition of various materials (i.e., organic, inorganic, and hybrid components), producing a variety of monodisperse functional particles. Moreover, the solvent-dependent disassembly of the supramolecular networks enables their removal, generating a wide range of corresponding hollow structures including capsules and yolk–shell structures. The versatility of these supramolecular networks, combined with their negligible cytotoxicity provides a pathway for the rational design of a range of particle systems (including core–shell, hollow, and yolk–shell) with potential in biomedical and environmental applications.

Hybrid conformal coatings-such as metal-phenolic networks (MPNs) that are constructed from the coordination-driven assembly of natural phenolic ligands-are of interest in areas including biomedicine, separation, and energy. To date, most MPN coatings have been prepared by immersing substrates in solutions containing the phenolic ligands and metal ions, which is a suitable method for coating small or flexible objects. In contrast, more industrially relevant methods for coating and patterning large substrates, such as spray assembly, have been explored to a lesser extent toward the fabrication of MPNs, particularly regarding the effect of process variables on MPN growth. Herein, a spray assembly method was used to fabricate MPN coatings with various phenolic building blocks and metal ions, and their formation and patterning were explored for different applications. Different process parameters including solvent, pH, and metal-ligand pair allowed for control over the film properties such as 2 thickness and roughness. Based on these investigations, a potential route for the formation of spray-assembled MPN films was proposed. Conditions favoring the formation of bis complexes could produce thicker coatings than those favoring the formation of mono or tris complexes. Finally, the spray-assembled MPNs were used to generate superhydrophilic membranes for oil-water separation and colorless films for UV shielding. The present study provides insights into the chemistry of MPN assembly and holds promise for advancing the fabrication of multifunctional hybrid materials.

Particle‐based pulmonary delivery has great potential for delivering inhalable therapeutics for local or systemic applications. The design of particles with enhanced aerodynamic properties can improve lung distribution and deposition, and hence the efficacy of encapsulated inhaled drugs. This study describes the nanoengineering and nebulization of metal–phenolic capsules as pulmonary carriers of small molecule drugs and macromolecular drugs in lung cell lines, a human lung model, and mice. Tuning the aerodynamic diameter by increasing the capsule shell thickness (from ≈100 to 200 nm in increments of ≈50 nm) through repeated film deposition on a sacrificial template allows precise control of capsule deposition in a human lung model, corresponding to a shift from the alveolar region to the bronchi as aerodynamic diameter increases. The capsules are biocompatible and biodegradable, as assessed following intratracheal administration in mice, showing >85% of the capsules in the lung after 20 h, but <4% remaining after 30 days without causing lung inflammation or toxicity. Single‐cell analysis from lung digests using mass cytometry shows association primarily with alveolar macrophages, with >90% of capsules remaining nonassociated with cells. The amenability to nebulization, capacity for loading, tunable aerodynamic properties, high biocompatibility, and biodegradability make these capsules attractive for controlled pulmonary delivery.