Beyond CO Storage: Enzyme-Amyloid Fibril Catalytic Hybrids for Long Cascade Reactions Converting CO into Fructose.

Enzyme immobilization is an efficient and cost-effective approach to recovering, stabilizing, and enhancing enzyme catalytic properties. It is a challenge, however, for coimmobilized multiple enzymes to perform consecutive reactions without being inactivated under similar conditions. Here, we present a facile enzyme immobilization platform using β-lactoglobulin amyloid fibril hydrogels.

Phase-separating peptide coacervates with programmable material properties for universal intracellular delivery of macromolecules.

Phase-separating peptides (PSPs) self-assembling into coacervate microdroplets (CMs) are a promising class of intracellular delivery vehicles that can release macromolecular modalities deployed in a wide range of therapeutic treatments. However, the molecular grammar governing intracellular uptake and release kinetics of CMs remains elusive. Here, we systematically manipulate the sequence of PSPs to unravel the relationships between their molecular structure, the physical properties of the resulting CMs, and their delivery efficacy.

Sustainable Smart Packaging from Protein Nanofibrils.

Smart packaging technologies are revolutionizing the food industry by extending shelf life and enhancing quality monitoring through environmental responsiveness. Here, a novel smart packaging concept is presented, based on amyloid fibrils (AM) and red radish anthocyanins (RRA), to effectively monitor food spoilage by color change. A protein nanofibrils biofilm is developed from whey protein, which is functionalized with RRA to endow the resulting films with advanced monitoring capabilities.

A structural rationale for reversible vs irreversible amyloid fibril formation from a single protein.

Reversible and irreversible amyloids are two diverging cases of protein (mis)folding associated with the cross-β motif in the protein folding and aggregation energy landscape. Yet, the molecular origins responsible for the formation of reversible vs irreversible amyloids have remained unknown. Here we provide evidence at the atomic level of distinct folding motifs for irreversible and reversible amyloids derived from a single protein sequence: human lysozyme.

Transitioning the production of lipidic mesophase-based delivery systems from lab-scale to robust industrial manufacturing following a risk-based quality by design approach augmented by artificial intelligence.

Lipidic mesophase drug carriers have demonstrated the capacity to host and effectively deliver a wide range of active pharmaceutical ingredients, yet they have not been as extensively commercialized as other lipid-based products, such as liposomal delivery systems. Indeed, scientists are primarily focused on investigating the physics of these systems, especially in biological environments. Meanwhile, the production methods remain less advanced, and researchers are still uncertain about how the manufacturing process might affect the quality of formulations.

Universality in the Structure and Dynamics of Water under Lipidic Mesophase Soft Nanoconfinement.

Water under soft nanoconfinement features physical and chemical properties fundamentally different from bulk water; yet, the multitude and specificity of confining systems and geometries mask any of its potentially universal traits. Here, we advance in this quest by resorting to lipidic mesophases as an ideal nanoconfinement system, allowing inspecting the behavior of water under systematic changes in the topological and geometrical properties of the confining medium, without altering the chemical nature of the interfaces. By combining Terahertz absorption spectroscopy experiments and molecular dynamics simulations, we unveil the presence of universal laws governing the physics of nanoconfined water, recapitulating the data collected at varying levels of hydration and nanoconfinement topologies.

Proteins for Applied and Functional Materials.

Shifting from a petroleum-based plastic society to a newer one built on circular economy principles requires maximizing the use of renewable resources and resolving the challenges that come with their use. Biopolymers have taken an important role in the design of biobased materials with functional properties, especially those derived from biomass available at a large scale. A number of recent studies have shown how proteins have a new dimension in developing functional materials, taking a step forward from their traditional use in food and biomedicine.

Hierarchical Protofilament Intertwining Rules the Formation of Mixed-Curvature Amyloid Polymorphs.

Amyloid polymorphism is a hallmark of almost all amyloid species, yet the mechanisms underlying the formation of amyloid polymorphs and their complex architectures remain elusive. Commonly, two main mesoscopic topologies are found in amyloid polymorphs characterized by non-zero Gaussian and mean curvatures: twisted ribbons and helical fibrils, respectively. Here, a rich heterogeneity of configurations is demonstrated on insulin amyloid fibrils, where protofilament packing can occur, besides the common polymorphs, also in a combined mode forming mixed-curvature polymorphs.

Cubosomes functionalized with antibodies as a potential strategy for the treatment of HER2-positive breast cancer.

Breast cancers that overexpress human epidermal growth factor receptor 2 (HER2) have poor prognosis. Moreover, available chemotherapies cause numerous side effects due to poor selectivity. To advance more effective and safer therapies for HER2-positive breast cancer, we explored the fusion of drug delivery technology and immunotherapy.

An evolutionarily conserved mechanism controls reversible amyloids of pyruvate kinase via pH-sensing regions.

Amyloids are known as irreversible aggregates associated with neurodegenerative diseases. However, recent evidence shows that a subset of amyloids can form reversibly and fulfill essential cellular functions. Yet, the molecular mechanisms regulating functional amyloids and distinguishing them from pathological aggregates remain unclear.

Synthesis of Bottlebrush Polymers with Spontaneous Self-Assembly for Dielectric Generators.

Cross-linked bottlebrush polymers received significant attention as dielectrics in transducers due to their unique softness and strain stiffening caused by their structure. Despite some progress, there is still a great challenge in increasing their dielectric permittivity beyond 3.5 and cross-linking them to defect-free ultrathin films efficiently under ambient conditions.

Single-site iron-anchored amyloid hydrogels as catalytic platforms for alcohol detoxification.

Constructing effective antidotes to reduce global health impacts induced by alcohol prevalence is a challenging topic. Despite the positive effects observed with intravenous applications of natural enzyme complexes, their insufficient activities and complicated usage often result in the accumulation of toxic acetaldehyde, which raises important clinical concerns, highlighting the pressing need for stable oral strategies. Here we present an effective solution for alcohol detoxification by employing a biomimetic-nanozyme amyloid hydrogel as an orally administered catalytic platform.

Single-Step Control of Liquid-Liquid Crystalline Phase Separation by Depletion Gradients.

Fine-tuning nucleation and growth of colloidal liquid crystalline (LC) droplets, also known as tactoids, is highly desirable in both fundamental science and technological applications. However, the tactoid structure results from the trade-off between thermodynamics and nonequilibrium kinetics effects, and controlling liquid-liquid crystalline phase separation (LLCPS) in these systems is still a work in progress. Here, a single-step strategy is introduced to obtain a rich palette of morphologies for tactoids formed via nucleation and growth within an initially isotropic phase exposed to a gradient of depletants.

Cation Triggered Self-Assembly of α-Lactalbumin Nanotubes.

Metal ions play a dual role in biological systems. Although they actively participate in vital life processes, they may contribute to protein aggregation and misfolding and thus contribute to development of diseases and other pathologies. In nanofabrication, metal ions mediate the formation of nanostructures with diverse properties.

The circular economy of water across the six continents.

Water is our most valuable and precious resource, yet it is only available in a limited amount. Sustainable use of water can therefore only operate in a circular way; nonetheless, still today depletion of water resources proceeds at an accelerated pace. Here, we quantitatively assess the water circular economy and the status of water management across 132 countries distributed over six continents by introducing the water circular economy index, WCEI, based on the three pillars of water circular economy, , decreasing, optimising, and retaining.

Hybrid Amyloid-Chitin Nanofibrils for Magnetic and Catalytic Aerogels.

In the quest for a sustainable and circular economy, it is essential to explore environmentally friendly alternatives to traditional petroleum-based materials. A promising pathway toward this goal lies in the leveraging of biopolymers derived from food waste, such as proteins and polysaccharides, to develop advanced sustainable materials. Here, we design versatile hybrid materials by hybridizing amyloid nanofibrils derived by self-assembly of whey, a dairy byproduct, with chitin nanofibrils exfoliated from the two distinct allomorphs of α-chitin and β-chitin, extracted from seafood waste.

From Soy Waste to Bioplastics: Industrial Proof of Concept.

The global plastic waste problem is pushing for the development of sustainable alternatives, encouraged by stringent regulations combined with increased environmental consciousness. In response, this study presents an industrial-scale proof of concept to produce self-standing, transparent, and flexible bioplastic films, offering a possible solution to plastic pollution and resource valorization. We achieve this by combining amyloid fibrils self-assembled from food waste with methylcellulose and glycerol.

Cholesteric Tactoids with Tunable Helical Pitch Assembled by Lysozyme Amyloid Fibrils.

Amyloid fibrils are biological rod-like particles showing liquid-liquid crystalline phase separation into cholesteric phases through a complex behavior of nucleation, growth, and order-order transitions. Yet, controlling the self-assembly of amyloids into liquid crystals, and particularly the resulting helical periodicity, remains challenging. Here, a novel cholesteric system is introduced and characterized based on hen egg white lysozyme (HEWL) amyloid fibrils and the results rationalized via a combination of experiments and theoretical scaling arguments.

Gold Recovery from E-Waste by Food-Waste Amyloid Aerogels.

Demand for gold recovery from e-waste grows steadily due to its pervasive use in the most diverse technical applications. Current methods of gold recovery are resource-intensive, necessitating the development of more efficient extraction materials. This study explores protein amyloid nanofibrils (AF) derived from whey, a dairy industry side-stream, as a novel adsorbent for gold recovery from e-waste.

Surface Cross-Linking by Macromolecular Tethers Enhances Virus-like Particles' Resilience to Mucosal Stress Factors.

Virus-like particles (VLPs) are emerging as nanoscaffolds in a variety of biomedical applications including delivery of vaccine antigens and cargo such as mRNA to mucosal surfaces. These soft, colloidal, and proteinaceous structures (capsids) are nevertheless susceptible to mucosal environmental stress factors. We cross-linked multiple capsid surface amino acid residues using homobifunctional polyethylene glycol tethers to improve the persistence and survival of the capsid to model mucosal stressors.

Expanding the Enzymatic Polymerization Landscape by Lipid Mesophase Soft Nanoconfinement.

Soft nanoconfinement can increase chemical reactivity in nature and has therefore led to considerable interest in transferring this universal feature to artificial biological systems. However, little is known about the underlying principles of soft nanoconfinement responsible for the enhancement of biochemical reactions. Herein we demonstrate how enzymatic polymerization can be expanded, optimized, and engineered when carried out under soft nanoconfinement mediated by lipidic mesophases.

Protein Nanotubes as Advanced Material Platforms and Delivery Systems.

Protein nanotubes (PNTs) as state-of-the-art nanocarriers are promising for various potential applications both in the food and pharmaceutical industries. Derived from edible starting sources like α-lactalbumin, lysozyme, and ovalbumin, PNTs bear properties of biocompatibility and biodegradability. Their large specific surface area and hydrophobic core facilitate chemical modification and loading of bioactive substances, respectively.

Food amyloid fibrils are safe nutrition ingredients based on in-vitro and in-vivo assessment.

Food protein amyloid fibrils have superior technological, nutritional, sensorial, and physical properties compared to native monomers, but there is as yet insufficient understanding of their digestive fate and safety for wide consumption. By combining SDS-PAGE, ELISA, fluorescence, AFM, MALDI-MS, CD, microfluidics, and SAXS techniques for the characterization of β-lactoglobulin and lysozyme amyloid fibrils subjected to in-vitro gastrointestinal digestion, here we show that either no noticeable conformational differences exist between amyloid aggregates and their monomer counterparts after the gastrointestinal digestion process (as in β-lactoglobulin), or that amyloid fibrils are digested significantly better than monomers (as in lysozyme). Moreover, in-vitro exposure of human cell lines and in-vivo studies with C.

Fast Probing Amyloid Polymorphism via Nanopore Translocation.

Neurodegenerative diseases are characterized by the presence of cross-β-sheet amyloid fibrils and a rich mesoscopic polymorphism, requiring noninvasive detection with high fidelity. Here, we introduce a methodology that can probe via a sensitive synthetic nanopore the complex polymorphism of amyloid fibrils by an automated and fast screening protocol. Statistically analyzing the translocation events on two model amyloid systems derived from β-lactoglobulin and lysozyme allows extracting the cross-sectional configuration of hydrated amyloid fibrils from current block amplitude and correlating dwell time with fibril length.