In this work, we present gel-in-gel water-in-oil (W/O) high internal phase emulsions (HIPEs) that feature high stability by structuring both phases of the emulsion. Compared to significant advances made in oil-in-water (O/ W) HIPEs, W/O HIPEs are extremely unstable and difficult to generate without introducing high concentrations of surfactants. Another main challenge is the low viscosity of both water and oil phases which promotes the instability of W/O HIPEs. Here, we demonstrate ultrastable W/O HIPEs that feature biphasic structuring, in which hydrogels are dispersed in oleogels, and self-forming, low-concentration interfacial Pickering crystals provide added stability. These W/O HIPEs exhibit high tolerance toward pH shock and destabilizing environments. In addition, this novel ultrastable gel-in-gel W/O HIPE is sustainable and made solely with natural ingredients without the addition of any synthetic stabilizers. By applying phase structuring within the HIPEs through the addition of various carrageenans and beeswax as structurants, we can increase the emulsion's stability and viscoelastic rheological properties. The performance of these gel-in-gel W/O HIPEs holds promise for a wide range of applications. As a proof of concept, we demonstrated herein the application as a gelled delivery system that enables the co-delivery of hydrophilic and hydrophobic materials at maximized loads, demonstrating high resistance to gastrointestinal pHs and a controlled-release profile.

Conventional delivery systems for hydrophilic material still face critical challenges toward practical applications, including poor retention abilities, lack of stimulus responsiveness, and low bioavailability. Here, we propose a robust encapsulation strategy for hydrophilic cargo to produce a wide class of aqueous core–shell–shell coconut-like nanostructures featuring excellent stability and multifunctionality. The numerous active groups (−SH, −NH2, and −COOH) of the protein–polysaccharide wall material enable the formation of shell-cross-linked nanocapsules enclosing a liquid water droplet during acoustic cavitation. A subsequent pH switch can trigger the generation of an additional shell through the direct deposition of non-cross-linked protein back onto the cross-linked surface. Using anthocyanin as a model hydrophilic bioactive, these nanocapsules show high encapsulation efficiency, loading content, tolerance to environmental stresses, biocompatibility, and high cellular uptake. Moreover, the composite double shells driven by both covalent bonding and electrostatics provide the nanocapsules with pH/redox dual stimuli-responsive behavior. Our approach is also feasible for any shell material that can be cross-linked via ultrasonication, offering the potential to encapsulate diverse hydrophilic functional components, including bioactive molecules, nanocomplexes, and water-dispersible inorganic nanomaterials. Further development of this strategy should hold promise for designing versatile nanoengineered core–shell–shell nanoplatforms for various applications, such as the oral absorption of hydrophilic drugs/nutraceuticals and the smart delivery of therapeutics.

Processing metal–organic frameworks (MOFs) into hierarchical macroscopic materials can greatly extend their practical applications. However, current strategies suffer from severe aggregation of MOFs and limited tuning of the hierarchical porous network. Now, a strategy is presented that can simultaneously tune the MOF loading, composition, spatial distribution, and confinement within various bio‐originated macroscopic supports, as well as control the accessibility, robustness, and formability of the support itself. This method enables the good dispersion of individual MOF nanoparticles on a spiderweb‐like network within each macrovoid even at high loadings (up to 86 wt %), ensuring the foam pores are highly accessible for excellent adsorption and catalytic capacity. Additionally, this approach allows the direct pre‐incorporation of other functional components into the framework. This strategy provides precise control over the properties of both the hierarchical support and MOF.

Copigmentation and encapsulation are the two most commonly used techniques for anthocyanin stabilization. However, each of these techniques by itself suffers from many challenges associated with the simultaneous achievement of color intensification and high stability of anthocyanins. Integrating copigmentation and encapsulation may overcome the limitation of usage of a single technique. This review summarizes the most recent studies and their challenges aiming at combining copigmentation and encapsulation techniques. The effective approaches for encapsulating copigmented anthocyanins are described, including spray/freeze‐drying, emulsification, gelation, polyelectrolyte complexation, and their combinations. Other emerging approaches, such as layer‐by‐layer deposition and ultrasonication, are also reviewed. The physicochemical principles underlying the combined strategies for the fabrication of various delivery systems are discussed. Particular emphasis is directed toward the synergistic effects of copigmentation and encapsulation, for example, modulating roles of copigments in the processes of gelation and complexation. Finally, some of the major challenges and opportunities for future studies are highlighted. The trend of integrating copigmentation and encapsulation has been just started to develop. The information in this review should facilitate the exploration of the combination of multistrategy and the fabrication of robust delivery systems for copigmented anthocyanins.

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In this work, we demonstrate sonochemically synthesized high internal phase emulsions (HIPEs), which feature high stability due to a permanent layer at the oil−water interface that nearly any material can form as long as it can be cross-linked during acoustic cavitation. Compared to conventional HIPEs prepared by homogenization emulsification, these ultrasonically prepared HIPEs exhibit excellent performance, including high tolerance to environmental shock (e.g., pH and surfactant) and excellent processability, as well as the capacity to structure liquid oil and provide controlled delivery for bioactive compounds. By changing the acoustic intensity, we can also easily tune the morphology, rheological properties, porosity, and closed-/open-cell structure of the porous materials. Furthermore, this unique type of HIPE is potentially sustainable because it can be stabilized solely by natural materials, such as proteins and polysaccharides, even at 0.5 wt %, without introducing any additional surfactants or synthetic particles. These findings suggest this sonochemical technique holds promise as a versatile, scalable, and environmentally friendly route for synthesizing ultrastable and fully natural HIPEs. Additionally, the material performance shown herein provides a proof-of-concept for the design of multifunctional HIPEs in various applications.

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