Search Results (74)

Although canna (Canna edulis Ker) starch possesses high swelling power, it remains an underutilized resource. This study aimed to engineer highly porous, food-grade canna starch aerogels as carriers for cyanidin-3-glucoside (C3G), incorporating enzymatically modified starch fractions prepared via α-amylase hydrolysis followed by lyophilization. Moderate enzymatic modification (sample AG1) effectively tailored the aerogel architecture by selectively removing amorphous regions. This targeted hydrolysis yielded a highly interconnected, hierarchical porous network with a high porosity (92%). Importantly, although this architectural transformation increased the average macroscopic pore size, it preserved mechanical integrity, as evidenced by a compressive strength exceeding 4000 kPa. In contrast, excessive hydrolysis led to pore collapse and structural failure. The AG1 aerogel exhibited a markedly enhanced C3G equilibrium adsorption capacity (43.9 mg/g), outperforming the native starch aerogel (36.0 mg/g). Adsorption data adhered to pseudo-second-order kinetics, indicating that this model provided a better description of the adsorption process, while the underlying adsorption mechanism may involve interactions between C3G and the aerogel matrix, potentially including hydrogen bonding. These results suggest that controlled enzymatically hydrolysis may provide a useful strategy for modulating the hierarchical microstructure of canna starch aerogels, thereby supporting their potential as effective carriers for sensitive bioactive compounds in functional food systems. Full article

Deep eutectic systems (DESs) have evolved from sustainable solvent alternatives to promising bioactive platforms with reported antimicrobial, anti-inflammatory, regenerative, cryoprotective, and cytoprotective properties. However, despite the growing number of biological studies, the mechanistic basis of these effects remains poorly understood because biological activity is still interpreted predominantly from the chemical identity of the hydrogen-bond donor and acceptor, rather than from the supramolecular organization of the eutectic system itself. This review is intended to provide anyone interested in the biomedical and pharmaceutical applications of DESs with a conceptual framework for understanding how supramolecular organization may influence the biological performance of DES-based systems, without requiring extensive expertise in physical chemistry. It critically analyzes the current evidence linking DES structure with biological function. The literature reveals that many reported biological responses cannot be fully explained by the properties of the individual constituents alone, supporting the existence of emergent physicochemical behavior associated with eutectic formation. Current evidence further demonstrates that DESs are dynamic supramolecular systems characterized by hydrogen-bond networks, nanoscale heterogeneity, hydration-dependent structural rearrangement, and persistent local organization under biologically relevant conditions. These structural features generate localized physicochemical microenvironments capable of modulating membrane organization, protein hydration, osmotic balance, and biomolecular interactions, providing a plausible mechanistic basis for the diverse biological effects reported to date. Our analysis also highlights a fundamental disconnect between the extensive physicochemical characterization of DESs and the predominantly composition-based interpretation of their biological activity. While conventional Quantitative Structure–Activity Relationship (QSAR) approaches rely on molecular descriptors of individual components, they fail to capture the higher levels of organization that characterize these dynamic multicomponent systems. Based on concepts established in supramolecular chemistry, self-assembled biomaterials, colloidal science, and soft matter, we propose a Hierarchical Structure–Activity Relationship (H-SAR) framework in which biological activity emerges from successive levels of organization extending from molecular composition and hydrogen-bond networks to nanostructural organization, hydration-dependent restructuring, localized physicochemical microenvironments, and biological interfaces. This framework provides a mechanistic basis for interpreting DES bioactivity and could offer a conceptual roadmap for the rational design, predictive modeling, and biomedical translation of next-generation bioactive deep eutectic systems. Full article

Flexible piezoresistive sensors are highly desirable for wearable health monitoring, yet balancing ultrahigh sensitivity and wide pressure detection range is a major bottleneck restricting their applications in electronic skin and soft robots. This work constructs a hierarchical piezoresistive sensor through a simple three-step fabrication: electrospinning PVDF/PAN fiber networks, polydopamine (PDA) surface modification, and in situ polypyrrole (PPy) polymerization for conductive sensing layers. As a dual-function interlayer, PDA forms hydrogen and covalent bonds with PPy to yield uniform, firm conductive coatings. The link between PPy morphology and sensing performance is clarified by regulating polymerization parameters. At a pyrrole concentration of 3 g/L, the optimized sensor achieves a high sensitivity of 220.88 kPa⁻¹ (0–10 kPa) and stable linear signals up to 1 MPa, with superior cycling durability over 5000 cycles and good biocompatibility. This scalable fabrication resolves the sensitivity–range tradeoff, promising wearable medical monitoring and human–machine interaction devices. Full article

Thermochemical conversion of nitrogen- and sulfur-rich biomass-derived wastes, such as sewage sludge, algae, and agricultural residues, is a promising route for renewable fuel production and waste valorization. However, fuel-bound nitrogen can be released as NH₃, HCN, and HNCO, while sulfur species such as H₂S, SO₂, and COS accelerate catalyst deactivation and generate NO_x/SO_x precursors. Metal-loaded ZSM-5 catalysts are attractive for clean catalytic pyrolysis because they combine the MFI pore confinement and tunable Brønsted/Lewis acidity of ZSM-5 with the hydrogen transfer, dehydrogenation, cracking, redox, and sulfur-tolerance functions of metal species. This review critically summarizes recent advances in metal-loaded ZSM-5 catalysts for catalytic denitrogenation of biomass-derived solid wastes. The formation and migration of NH₃, HCN, HNCO, tar-N, and char-N are first discussed to clarify the chemical basis of fuel-N conversion. The effects of ZSM-5 pore structure, acid-site distribution, Si/Al ratio, hierarchical porosity, and synergy on adsorption, diffusion, C-N bond cleavage, heterocyclic-N ring-opening, aromatization, and nitrogen redistribution are then analyzed. Catalyst deactivation under realistic pyrolysis atmospheres is also highlighted, including coke deposition, metal sintering, framework dealumination, mineral poisoning, and H₂S/SO₂/COS-induced sulfur poisoning. Finally, future directions are proposed for designing multifunctional ZSM-5-based catalysts integrating denitrogenation activity, sulfur resistance, coke resistance, regenerability, and quantitative nitrogen/sulfur mass balance. Full article

Driven by the rising frequency of extreme climatic events and the escalating demand for sustainable infrastructure, modern pavement materials must deliver enhanced resilience, structural stability, and environmental adaptability. This study presents the design and synthesis of a novel polyurethane-polyurea (PU-PUa) pavement binder, engineered via a synergistic framework combining nanoscale microphase separation and a hierarchical hydrogen-bonding network. Utilizing a streamlined, one-step synthesis approach involving an aliphatic isocyanate, a polyaspartic ester, polytetramethylene ether glycol, and 1,4-butanediol, the PU-PUa copolymer achieves distinct nanoscale phase separation between its hard and soft segments. Fourier transform infrared (FTIR) spectroscopy verifies the successful formation of characteristic PU-PUa moieties and a multi-scale hydrogen-bonding network, while DSC and DMA reveal SSC-dependent soft-segment mobility, crystallization/melting behavior, and viscoelastic relaxation. These intra- and inter-segmental interactions, together with thermally activated soft-segment transitions, establish the structural foundation for the macro-performance enhancement of the system. Comprehensive evaluations demonstrate that the PU-PUa binder exhibits excellent mechanical and highly tunable properties. Rheological measurements indicate that increasing the soft segment content (SSC) or incorporating an appropriate diluent concentration significantly lowers the system viscosity, thereby enhancing processing workability during mixing and paving. Contact angle goniometry reveals that the surface hydrophobicity of PU-PUa can be effectively regulated by adjusting the SSC, offering a viable strategy to optimize moisture damage resistance. Moreover, curing behavior analyses show that the polymerization kinetics are strictly governed by both the SSC and environmental temperature, where a lower SSC or elevated curing temperature accelerates strength development. Mechanically, the PU-PUa binder displays desirable surface hardness (>80 Shore A) and exceptional aggregate adhesion (>2 MPa), ensuring robust bonding stability and resistance to traffic-induced abrasion. Characterized by balanced tensile performance, the elongation at break of the binder can be tailored from 90% to 161%, while its tensile strength varies between 6.4 MPa and 17.8 MPa at intermediate temperatures, manifesting excellent resilience and cracking resistance. Overall, this molecular-to-macroscopic design strategy establishes the PU-PUa copolymer as a highly promising, durable binder for next-generation resilient pavement infrastructures. Full article

Microplastics (MPs, plastic particles < 5 mm) and nanoplastics (NPs, plastic particles generally <1 µm), collectively referred to as micro/nanoplastics (MNPs), have emerged as critical contaminants in wastewater systems due to their persistence, small size, and ability to act as vectors for co-contaminants. Conventional wastewater treatment technologies are often insufficient for the effective removal of microplastics, particularly for smaller particles and nanoplastics, necessitating the development of functional materials and innovative treatment strategies. In this review, recent advances in carbon-based materials, cellulose-based materials, and their hybrid carbon–cellulose composites for microplastics removal are critically analyzed and comparatively discussed. Particular attention is given to the structure–function relationships governing adsorption performance, including the roles of hierarchical porosity, surface chemistry, and interfacial interactions. The key mechanisms responsible for microplastics capture—such as hydrophobic interactions, π–π stacking, hydrogen bonding, electrostatic attraction, physical entrapment, and pore trapping—are systematically discussed. Carbon–cellulose composite materials are highlighted as a promising class of multifunctional adsorbents due to their synergistic combination of hydrophilic cellulose scaffolds and hydrophobic carbon domains. This dual functionality enables efficient removal of microplastics across a wide range of sizes and morphologies. Recent developments in magnetic and superhydrophobic composite systems further demonstrate enhanced separation efficiency, recyclability, and potential applicability in real wastewater environments. In addition to summarizing recent progress, this review critically examines the methodological inconsistencies, mechanistic uncertainties, and practical limitations associated with current adsorption systems. Despite significant progress, several challenges remain, including the lack of standardized evaluation methods, limited validation under real wastewater conditions, material stability issues, and scalability constraints. Future research directions are proposed, focusing on rational material design, sustainable carbon sources, multifunctional hybrid systems, and integration into existing treatment infrastructures. The development of sustainable hybrid adsorption systems for microplastics remediation also contributes to the achievement of Sustainable Development Goal 6 (Clean Water and Sanitation) by supporting improved wastewater treatment technologies and reduction in emerging aquatic contaminants. Full article

Growing environmental concerns associated with non-renewable and persistent materials have intensified the search for sustainable alternatives, with cellulosic fibers and nanocellulose emerging as promising candidates. This review examines diverse product opportunities where interdigitation plays a critical role, including nanopaper and barrier films, wet wipe technologies, spun cellulose-based yarns, hydrogels, and composite materials. Particular emphasis is placed on the interplay between colloidal stability, fibrillar alignment, hydrogen bonding, and time-dependent network evolution in governing material performance. Additionally, emerging strategies such as hydroentanglement, ice-templating, in situ crosslinking, and post-formation modification are discussed as means to optimize interdigitated structures. The article further explores how conventional papermaking processes may be reimagined to better exploit interdigitation through innovations in fiber dispersion, alignment, and controlled crosslinking. Interdigitation is presented not as a discrete processing tool but as a unifying framework for understanding and engineering hierarchical cellulose networks. By leveraging the inherent fibrillar nature of cellulose and the dynamics of self-assembly, this paradigm offers new pathways towards the development of next-generation, high-performance, bio-based products that contribute to a circular economy. Full article

Self-healing materials have attracted increasing attention as a strategy to enhance durability, extend service life, and reduce maintenance in advanced material systems. Among these, cellulose-based self-healing materials represent a sophisticated intersection between sustainable macromolecular chemistry and adaptive materials science. This review provides a synthesis of recent advancements in the field, systematically categorizing materials derived from cellulose raw materials. We evaluate the fundamental chemical strategies employed to achieve autonomous repair, distinguishing between extrinsic mechanisms—utilizing cellulose-based micro/nano-capsules to sequester healing agents—and intrinsic mechanisms governed by dynamic covalent chemistry (Schiff-base, boronic ester, Diels–Alder) and supramolecular interactions (hydrogen bonding, metal–ligand coordination, and host–guest assemblies). The analysis highlights how cellulose’s hierarchical structure and abundant surface functionality are leveraged to overcome the traditional trade-off between mechanical toughness and healing efficiency. Particular emphasis is placed on the transition from simple structural hydrogels to sophisticated multifunctional systems. These include ultra-stretchable strain and pressure sensors for e-skin applications, biocompatible and injectable matrices for chronic wound management and stem cell delivery, and advanced anti-freezing eutectogels for performance in extreme environments. Furthermore, we explore the integration of cellulose into traditional sectors, such as self-healing concrete utilizing microbe-induced calcification and smart, eco-friendly coatings for corrosion protection. Finally, we discuss critical challenges, including environmental stability, scalability, and the development of standardized evaluation protocols, providing a roadmap for the next generation of bio-derived, sustainable and intelligent materials. Full article

Bone grafting remains limited, and the strategies to design even more structurally complex scaffolds—able to reproduce the hierarchical architecture of bone extracellular matrix—are rapidly growing. In this study, we report the fabrication of a hierarchically structured scaffold produced by layering poly(ε-caprolactone)/gelatin (PCL/Gt) or poly(lactic acid)/gelatin (PLA/Gt) electrospun nanofibers via coaxial electrospinning onto 3D-printed poly(lactic acid) (PLA) scaffolds via fused deposition modeling (FDM). After the printing process, PLA disks (10 × 1 mm, 20% infill, ~80% porosity, pore size ~1.57 mm) were coated with core/shell (PCL/Gt, PLA/Gt) fibers to investigate the in vitro interfacial response of osteoblasts in comparison with monocomponent fibrous coatings (PCL, PLA, Gt). SEM and TEM confirmed that core/shell fibers exhibited bead-free morphologies, with a significant reduction in fiber diameter (≈287–316 nm) and higher interfibrillar porosity compared to monocomponent fibers. FTIR and thermogravimetric analyses indicated the presence of hydrogen bonding between the polyester and gelatin, and the absence of residual solvent after deposition. At the same time, water contact angle measurements confirmed an increase in hydrophilic properties from 80–86° to 120° ascribable to the presence of gelatin. Accordingly, in vitro response of human fetal osteoblasts (hFOB 1.19) exhibited an evident improvement in the case of Gt-based fibrous coatings (i.e., PCL/Gt and PLA/Gt) in terms of early adhesion (4–24 h) and metabolic activity from 3 to 21 days, cell spreading into star-shaped morphologies, formation of extracellular matrix, and mineral phase deposition. In more detail, a remarkable increase in alkaline phosphatase activity was observed in Gt-based coaxial coatings from day 7 onward, with the highest values recorded for PLA/Gt. Overall, we demonstrated that the Gt-based coaxial fibrous coating provided a mix of topological and biochemical cues that synergistically promoted key osteoblast activities at the interface, supporting the regeneration of new bone tissue in highly tailored 3D-printed scaffolds, thus suggesting a promising strategy for personalized regenerative medicine. Full article

Zeolite-based composite nanomaterials represent a versatile and mechanistically rich platform for the removal of organic micropollutants (OMPs)—including pharmaceuticals, endocrine-disrupting compounds, pesticides, and per- and polyfluoroalkyl substances (PFAS)—from contaminated water systems. Although pristine zeolite frameworks provide well-defined microporous architectures, tunable Si/Al ratios, and ion-exchange capacity, their intrinsic hydrophilicity restricts interaction diversity and limits performance toward the structurally heterogeneous OMPs prevalent in real aquatic environments. Composite integration with carbonaceous nanophases, functional polymers and surfactants, and catalytically active metal oxide nanoparticles substantially extends this interaction repertoire, yielding multifunctional materials whose adsorption performance exceeds that of the individual components. Drawing on a systematic survey of peer-reviewed literature published between 2016 and 2026, this review develops a mechanism-oriented, structure–property–performance framework examining five dominant adsorption mechanisms—electrostatic attraction, π–π stacking, hydrogen bonding, hydrophobic partitioning, and micropore confinement—in relation to composite nanoarchitecture, surface chemistry, and structural parameters. The modulating influence of realistic water matrix conditions on adsorption efficiency is critically assessed, alongside challenges of regeneration, long-term stability, metal leaching, and the persistent gap between laboratory-scale synthesis and scalable deployment. Priority research directions are identified, including standardized performance evaluation under environmentally representative conditions and rational design of hierarchical multifunctional nanocomposites from earth-abundant and waste-derived precursors. Full article

To overcome graphene aggregation in aqueous nanofluids, polycarboxylate-modified structural graphene (PSG) was synthesized via surface functionalization. Characterizations indicate that the modification preserves the 3D hierarchical porous framework while ensuring exceptional dispersion stability through steric hindrance and enhanced hydrophilicity. Convective heat transfer evaluations demonstrated remarkable enhancement; notably, the 0.1 wt% PSG nanofluid achieved a 46% increase in the heat transfer coefficient over pure water at Re = 4000. Molecular dynamics simulations further revealed the underlying interfacial mechanisms. The surface-anchored oxygen-containing groups induce a dense, hydrogen-bonded hydration layer that restricts local water diffusion. This highly ordered interfacial structure may facilitate vibrational energy exchange across the solid–liquid boundary. Together with the intrinsic high-conductivity 3D skeleton, these microscopic interactions are likely to contribute to the enhanced macroscopic thermal performance, providing a promising framework for designing advanced graphene-based thermal management fluids. Full article

Microwave-assisted pyrolysis (MAP) has emerged as a revolutionary technology for converting solid waste into high-value hydrocarbons. However, conventional pyrolysis and traditional single-function catalysts often face an inevitable “performance trade-off” involving severe mass transfer resistance, poor microwave absorption, and rapid coking. This review systematically summarizes the recent evolution of catalyst design toward advanced multi-site composites. It highlights the synergistic mechanisms of integrating microwave-responsive cores, hierarchical pore networks, and metal-acid bifunctional sites to achieve ultrafast localized heat transfer, targeted bond cleavage, and in-situ coking suppression. Furthermore, this paper critically examines current bottlenecks in scaling MAP to industrial levels. To address these challenges, we discuss emerging solutions, including hydrogen-enriched co-pyrolysis, non-destructive in-situ regeneration, and the integration of machine learning frameworks for intelligent process optimization. Full article

This study prepared alkali-modified porous biochar (KABC-1h) from straw via KOH impregnation and pyrolysis and systematically investigated its adsorption performance toward tetracycline (TC) in water. The optimal modification condition was determined as 2 mol/L KOH impregnation for 1 h followed by pyrolysis at 600 °C. Characterization results showed that alkali modification significantly increased the BET-specific surface area to 132.56 m²/g, enriched hierarchical micro-mesoporous structure, and introduced abundant oxygen-containing functional groups. The maximum adsorption capacity of KABC-1h for TC reached 21.60 mg/g, much higher than 14.11 mg/g of unmodified biochar (BC). Adsorption kinetics followed the pseudo-second-order model well, revealing that chemisorption dominated the rate-controlling step. Adsorption isotherms fitted the Freundlich model better, indicating multilayer heterogeneous adsorption on the biochar surface. Mechanism studies confirmed that TC adsorption was realized mainly through hydrogen bonding, π-π interaction, and surface complexation, whereas electrostatic interaction played a minor role. Moreover, KABC-1h exhibited stable adsorption efficiency over a wide pH range (4.5–11.5) and strong anti-interference ability against coexisting ions, with 59.0% removal efficiency retained after three regeneration cycles. This work demonstrates that KOH-modified porous biochar is a promising adsorbent for efficient TC removal from aqueous solution, providing a feasible strategy for agricultural waste valorization and antibiotic wastewater treatment. Full article

This work reports on the synthesis and electrochemical investigation of sustainable carbon–TiO₂ nanocomposites derived from marine biowaste, designed to elucidate light-assisted charge storage mechanisms in non-aqueous electrolytes. Porous carbons obtained from prawn chitin and blue shark gelatin were decorated in situ with TiO₂ nanoparticles using a deep eutectic solvent (DES) as a green synthesis medium. Structural and morphological characterisation revealed that TiO₂ incorporation induces significant nanoscale reorganisation of the carbon framework, resulting in hierarchical porosity, increased surface area, and intimate semiconductor–carbon interfaces. Electrochemical evaluation in a three-electrode configuration using an ethaline-based DES electrolyte demonstrated that TiO₂ decoration substantially enhances capacitive performance and cycling stability, with the prawn chitin-derived composite achieving a specific capacitance of 54 ± 3 F g⁻¹ and 91% retention after 10,000 cycles. Under illumination, all TiO₂-containing composites exhibited a pronounced increase in anodic current response and discharge time, indicating photo-assisted surface charge accumulation. Although the absolute capacitance values are modest compared to those of aqueous supercapacitor systems, the results provide mechanistic insight into the interplay among nanostructure, semiconductor photoactivity, and ion transport in viscous, hydrogen-bonded DES electrolytes. By combining waste-derived carbons, green synthesis routes, and photo-responsive nanostructures, this study highlights a sustainable strategy for developing multifunctional carbon-based nanomaterials with light-modulated electrochemical behaviour. Full article

Electrolysis of water is a promising emission-free approach of hydrogen production, making water electrolyzers important for many renewable energy systems. Electrochemical electrodes enriched with nanocatalysts can significantly advance such technologies, but the use of nanomaterials, deployed as packed powders or painted films, is generally limited by durability and reusability challenges. To overcome these deficiencies, we have fabricated hierarchical hybrid electrode (HHE) monoliths comprising carpet-like arrays of multiwalled carbon nanotubes covalently bonded to porous reticulated carbon foams that are further functionalized with strongly attached nanocatalysts. This paper presents our investigation of HHE materials with CNT carpets and palladium nanoparticle (PdNP) catalysts in two key electrolysis reactions: hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Their performances in different electrolytes have been evaluated using cyclic voltammetry, linear sweep voltammetry and Tafel analysis. This architecture provided multi-faceted advantages, and the contribution of each nanocomponent in the monolith has been analyzed. The presence of Pd-NP in the HHE also improved the electrode’s tolerance to Cl⁻ ions, which is very promising for saline water electrolysis. These studies indicate that the HHE architecture of electrochemical electrodes can be a versatile and tunable option for future electrochemical systems relevant to renewable energy applications. Full article