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The highly efficient utilization of bioresources and natural organic wastes has attracted great attention, due to the high-speed consumption and shortage of energy in modern society. Aerogels, attributable to their outstanding properties and potential applications in diverse fields, have been a major topic of innovative materials research in the last decades. While previously the scientific community has mainly focused on inorganic- and plastic-based aerogels, recent years have witnessed a growing interest in their biomass-based counterparts. In fact, numerous studies on the fabrication, modification, and applications of cellulose, polysaccharide, protein, peptide, and other bio-derived aerogels have been widely reported. In this review, we focus on recent advances in the biomass-based aerogels field. The analysis that we perform ranges from their structural design to routes for functional tailoring, and encompasses resource-efficient applications; the aim is to provide a comprehensive review based on a robust analysis of available data. The fabrication techniques, structure and properties of biomass-based aerogels are introduced, together with their chemical, mechanical, electrical, optical, and biological properties. In addition, the structural design, functional tailoring, and applications of biomass-based aerogels are demonstrated. Furthermore, we enrich the actual literature state-of-the-art with a broad sustainability analysis, that compares biomass-based aerogels to the most studied inorganic/plastic-based counterparts. To this end, we perform a comparison with inorganic- and plastic-based aerogels by sustainability footprint analysis, which accounts for 12 sustainability parameters on environmental, social, and techno-economic impacts. This review will guide readers in understanding the fabrication of biomass-based aerogels, together with their structural and functional adjustment, through comprehensively presenting the state-of-the-art on their sustainable applications in fields as diverse as biomedical engineering, energy materials, nanodevices, chemical engineering, and environmental science., Progress in materials science, 125, ISSN:0079-6425, ISSN:1873-2208

β-Lactoglobulin amyloid fibrils are bio-colloids of high interest in many fields (e.g. water purification, cell growth, drug delivery and sensing). While the mechanical properties of pure amyloid fibril gels meet the needs of some applications, mechanical fragility often hinders a wider usage basin. In this work, we present a simple and sustainable approach for reinforcing amyloid fibril hydrogels and aerogels, upon the diffusion of polysaccharides (low-acetylated Gellan Gum and κ-carrageenan) inside their mesh. The formed hybrid materials show enhanced resistance upon compression, without any loss of the exquisite surface reactivity of the amyloid fibrils. The proposed approach can pave the way for designing composite materials that are both highly functional and environmentally friendly.

The fundamental understanding of the gelation kinetics, stress relaxation and temporal evolution in colloidal filamentous gels is central to many aspects of soft and biological matter, yet a complete description of the inherent complex dynamics of these systems is still missing. By means of photon correlation imaging (PCI), we studied the gelation of amyloid fibril solutions, chosen as a model filamentous colloid with immediate significance to biology and nanotechnology, upon passage of ions through a semi-permeable membrane. We observed a linear-in-time evolution of the gelation front and rich rearrangement dynamics of the gels, the magnitude and the spatial propagation of which depend on how effectively electrostatic interactions are screened by different ionic strengths. Our analysis confirms the pivotal role of salt concentration in tuning the properties of amyloid gels, and suggests potential routes for explaining the physical mechanisms behind the linear advance of the salt ions., Soft Matter, 18 (30), ISSN:1744-683X, ISSN:1744-6848

Mesh size is a crucial parameter that governs the behavior of gels made of semiflexible polymers. We show that the average mesh size of amyloid fibril gels can be extracted from simple dynamic ligh...

Amyloid functional materials from amyloid fibril building blocks, produced in vitro from amyloidogenic natural proteins or synthetic peptides, show diverse functionalities ranging from environmental science and biomedicine, to nanotechnology and biomaterials. However, sustainable and affordable sources of amyloidogenic proteins remain the bottleneck for large-scale applications, and to date, interest remains essentially limited to fundamental studies. Plant-derived proteins would be an ideal source due to their natural abundance and low environmental impact. Hereby oat globulin, the primary protein of oat plant (Avena sativa), is utilized to yield high-quality amyloid fibrils and functional materials based thereof. These fibrils show a rich multistranded ribbon-like polymorphism and a fibrillization process with both irreversible and reversible pathways. The authors furthermore fabricate oat-amyloid aerogels, films, and membranes for possible use in water purification, sensors, and patterned electrodes. The sustainability footprint of oat-amyloids against other protein sources is demonstrated, anticipating an environmentally-efficient platform for advanced materials and technologies., Advanced Science, 9 (4), ISSN:2198-3844

Water contamination is a global threat due to its damaging effects on the environment and human health. Water pollution by microplastics (MPs), dissolved natural organic matter (NOM), and other turbid particles is ubiquitous in water treatment. Here, we introduce lysozyme amyloid fibrils as a novel natural bio-flocculant and explore their ability to flocculate and precipitate the abovementioned undesired colloidal objects. Thanks to their positively charged surface in a very broad range of pH, lysozyme amyloid fibrils show an excellent turbidity removal efficiency of 98.2 and 97.9% for dispersed polystyrene MPs and humic acid (HA), respectively. Additionally, total organic carbon measurements confirm these results by exhibiting removal efficiencies of 93.4 and 61.9% for purifying water from dispersed MPs and dissolved HA, respectively. The comparison among amyloid fibrils, commercial flocculants (FeCl3 and polyaluminumchloride), and native lysozyme monomers points to the superiority of amyloid fibrils at the same dosage and sedimentation time. Furthermore, the turbidity of pristine and MP-spiked wastewater and lake water decreased after the treatment by amyloid fibrils, validating their coagulation-flocculation performance under natural conditions. All these results demonstrate lysozyme amyloid fibrils as an appropriate natural bio-flocculant for removing dispersed MPs, NOM, and turbid particles from water.

Solar distillation is an appealing and facile technology for seawater desalination and water purification, but constructing stable, environmentally-friendly, and cost-effective solar evaporators often remain unfeasible. Here, amyloid hybrid aerogels are introduced for universal and renewable freshwater production by relying on the combination of sustainable materials and solar energy, thus making the process highly ecological and virtually costless. Amyloid fibrils obtained from whey, a byproduct of the dairy industry, are used as the main scaffold for the aerogels, whose solar energy harvesting properties of the top surface are enhanced by bioinspired dark polymers, such as polydopamine. Due to the fast water transport throughout the porous aerogels, the high-yielding photothermal conversion ability of the top surface, and efficient heat insulation at the bottom, the hybrid amyloid fibrils aerogel exhibits a water evaporation rate of 1.61 kg center dot m(-2) h(-1) with a solar-thermal conversion efficiency as high as 91.3% under 1 sun illumination. The process allows desalinating various seawater sources with different salinities to levels below the drinking water threshold recommended by the World Health Organization. Moreover, the same hybrid amyloid evaporator is highly efficient in removing heavy metals, organic pollutants, bacteria, and viruses from water, introducing a general, sustainable and energy-efficient solution for desalination and water purification., Advanced Sustainable Systems, 6 (1)

Physical interactions between vascular endothelial growth factor (VEGF), a central player in blood endothelial cell biology, and fibronectin, a major fibrillar protein of the extracellular matrix, are important determinants of angiogenic activity in health and disease. Conditions signaling the need for new blood vessel growth, such as hypoxia and low extracellular pH, increase VEGF–fibronectin interactions. These interactions can be further fine-tuned through changes in the availability of the VEGF-binding sites on fibronectin, regulated by conformational changes induced by heparin and heparan sulfate chains within the extracellular matrix. These interactions may alter VEGF bioavailability, generate gradients, or alter the way VEGF is recognized by and activates its cell-surface receptors. Here, using equilibrium and kinetic studies, we discovered that fibronectin can also interact with the extracellular domain of the VEGF receptor 2 (VEGFR2). The VEGFR2-binding sites on fibronectin show great similarity to the VEGF-binding sites, as they were also exposed upon heparin-induced conformational changes in fibronectin, and the interaction was enhanced at acidic pH. Kinetic parameters and affinities for VEGF and VEGFR2 binding to fibronectin were determined by surface plasmon resonance measurements, revealing two populations of fibronectin-binding sites for each molecule. Our data also suggest that a VEGF/VEGFR2/fibronectin triple complex may be formed by VEGF or VEGFR2 first binding to fibronectin and subsequently recruiting the third binding partner. The formation of such a complex may lead to the activation of distinct angiogenic signaling pathways, offering new possibilities for clinical applications that target angiogenesis., Journal of Biological Chemistry, 296, ISSN:0021-9258, ISSN:1083-351X

Niemann-Pick Disease Type C (NPC) is a severe neurovisceral disorder that is pathophysiologically characterized by intracellular transport abnormalities leading to cytoplasmic accumulation of lipids such as cholesterol and multiple sphingolipids, including sphingosine. The compound 2-hydroxypropyl-β-cyclodextrin (HPβCD) is a compound with high cholesterol complexation capacity and is currently under clinical investigation for the treatment of NPC. However, due to its short blood half-life, high doses are required to produce a therapeutic effect. It has been reported in mice that HPβCD’s circulation time and efficacy can be improved by increasing its size via polymerization, but the biodegradable nature of these systems did not allow the contribution of the macromolecule to the activity to be determined. In this work, stable forms of polymerized HPβCD were generated (via epichlorohydrin crosslinking) to investigate their in vitro mechanisms of action and in vivo effects. Crosslinked CDs (8-312 kDa) displayed a 10-fold greater complexation capacity towards cholesterol than monomeric HPβCD but were taken up by cells to a lower extent (in a size-dependent fashion), resulting in an overall comparable in vitro effect on intracellular cholesterol accumulation that was dependent on cholesterol complexation. When tested in vivo, the crosslinked 19.3 kDa HPβCD exhibited a longer terminal half-life than the monomeric HPβCD. However, it did not increase the life span of Npc1 mice, possibly due to reduced organ penetration and brain diffusion consequence of its large molecular weight. This could be circumvented by the application of magnetic resonance imaging-guided low intensity-pulsed focused ultrasound (MRIg-FUS), which increased the brain penetration of the CD. In conclusion, stable forms of polymerized HPβCD constitute valuable tools to elucidate CDs’ mechanism of action. Moreover, the use of MRIg-FUS to maximize CDs tissue penetration warrants further investigation, as it may be key to harnessing CDs full therapeutic potential in the treatment of NPC.Graphical abstractThe 2-hydroxypropyl-β-cyclodextrin (HPβCD) is a well-established pharmaceutical excipient that can complex cholesterol and is currently under clinical investigation to treat Niemann-Pick Disease Type C (NPC). However, high doses of the drug are needed to achieve a therapeutic effect. Using stable and long circulating crosslinked HPβCDs, this study attempts to further understand the mechanisms behind CDs’ activity.