Malleable, Ultrastrong Antibacterial Thermosets Enabled by Guanidine Urea Structure

Advanced Science, Год журнала: 2024, Номер 11(30)

Опубликована: Июнь 13, 2024

Abstract Dynamic covalent polymers (DCPs) that strike a balance between high performance and rapid reconfiguration have been challenging task. For this purpose, solution is proposed in the form of new dynamic supramolecular motif—guanidine urea structure (GUAs). GUAs contain complex diverse chemical structures as well unique bonding characteristics, allowing guanidine to demonstrate advanced physical properties. Noncovalent interaction aggregates (NIAs) confirmed GUA‐DCPs through multistage H‐bonding π‐π stacking, resulting an extremely Young's modulus 14 GPa, suggesting remarkable mechanical strength. Additionally, guanamine linkages GUAs, type bond, provide resins with excellent malleability reprocessability. Guanamine metathesis validated using small molecule model compounds, temperature dependent infrared rheological behavior following dissociative exchange mechanism. Moreover, inherent photodynamic antibacterial properties are extensively verified by experiments. Even after undergoing three reprocessing cycles, rate remains above 99% 24 h, highlighting their long‐lasting effectiveness. nature, tuneable composition, combination make them promising candidates for various technological advancements.

Язык: Английский

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Towards Sustainable Materials: A Review of Acylhydrazone Chemistry for Reversible Polymers

Chemistry - A European Journal, Год журнала: 2024, Номер 30(49)

Опубликована: Июнь 18, 2024

Transitioning towards a circular economy, extensive research has focused on dynamic covalent bonds (DCBs) to pave the way for more sustainable materials. These enable debonding and rebonding demand, as well facilitating end-of-life recycling. Acylhydrazone/hydrazone chemistry offers material with high stability under neutral basic conditions making it promising candidate materials research, though is susceptible acid degradation. However, this degradation acidic can be exploited, widely applicable in self-healing biomedical fields, potential reprocessing This review highlights studies exploring reversibility of acylhydrazone/hydrazone various polymers, altering their properties, utilizing them applications such self-healing, reprocessing, The also focuses how mechanical properties are affected by presence linkages, methods improve performance.

Язык: Английский

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Integrating ex-ante and prospective life-cycle assessment for advancing the environmental impact analysis of emerging bio-based technologies

Sustainable Production and Consumption, Год журнала: 2023, Номер 43, С. 319 - 332

Опубликована: Ноя. 18, 2023

Unlike the fossil-based alternatives, many emerging bio-based technologies are still at early lab or pilot scale and not representative of optimized industrial conditions. This makes a robust comparison their environmental performances via life-cycle assessment (LCA) challenging. We propose framework to combine scaling-up projections early-stage (ex-ante LCA) with influence future socio-economic scenarios (prospective LCA), using range new polymers produced from forest residues as case study. The combined takes step-by-step approach in modifying process inventories projecting them for impact assessment. In our study, climate change lab-scale processes decreases 105–471 kg CO2-eq./kg polymer 9–14 after application ex-ante LCA, highest reduction (83 %) coming identified synergies (e.g., solvent recovering). Combining prospective LCA additionally reduces up 56 % by 2050, relative results only. Other impacts decrease well, particularly freshwater eutrophication (up 99 reduction), photochemical oxidant formation (99 %), marine (98 %). secures more products conventional such it helps identification improvements both technological background supply chains that needed make systems outperform fossil counterparts. A consistent integration is instrumental prioritize research investments upscaling most promising sustainability perspective, ultimately guide sustainable transition towards circular bioeconomy.

Язык: Английский

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Mechanism Study on Synthesis of Biobased Polycarbonate from Diphenyl Carbonate and Isosorbide with Metal-Free Catalysts by Identifying Reactivity of endo-OH and exo-OH

ACS Sustainable Chemistry & Engineering, Год журнала: 2024, Номер 12(12), С. 5036 - 5045

Опубликована: Март 13, 2024

Isosorbide (ISB), a promising biobased monomer with two asymmetric hydroxyl groups, however, exhibits an unsatisfying reactivity in the poly(isosorbide carbonate) (PIC) synthesis metal-free catalysts. In this work, we employed density functional theory (DFT) calculations to address existing disputes surrounding catalytic mechanisms, focusing on potential reaction pathways catalyzed by tetraethylammonium hydroxide ([TEA][OH]). Energy profiles reveal that synergistic mechanism represents energetically favorable route for PIC synthesis. Meanwhile, disclose quaternary ammonium base as catalyst precursor phenol ([TEA][Ph]) acting effective cycle. Seeking enhanced efficiency, cation modification of was conducted, and hexadecyl trimethylammonium ([HTMA][OH]) exceptional performance low energy barriers 29.1 30.0 kcal/mol exo-OH endo-OH, respectively. This aligns kinetic experiments, emphasizing superior efficiency [HTMA][OH]. The proposed model enables accurate predictions terminal group distribution. A thorough examination steric hindrance electronic effect impact pathway during transesterification offers significant insights efficient design not only polyester but also chemical recycling strategy wasted ones.

Язык: Английский

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Biobased Self-healable Photoluminescent Polyacylhydrazones Imparted by Supramolecular Interactions

Macromolecules, Год журнала: 2025, Номер unknown

Опубликована: Янв. 13, 2025

With the rise of circular economy, self-healing polymers have attracted significant attention for their longer lifespan and greater recyclability compared with traditional thermoplastics thermosetting polymers. However, addressing instability units to develop high-performance materials remains a challenge. Herein, we report series superior polyimine derivatives, biobased polyacylhydrazones (bio-PHys), via aldehyde-hydrazide condensation. The coexistence amide bonds imine bonds, which provide hydrogen bonding dynamics, imparts remarkable mechanical properties (tensile strength 103 MPa, elongation at break 180%) bio-PHys, along notable capabilities under glass transition temperature (Tg). Bio-PHys also exhibits potential scalable production, excellent processability, photoluminescence characteristics. We explored its application in adhesive-free laminated substrates thoroughly investigated aggregation-induced emission acylhydrazone group. Furthermore, utilized bio-PHys create recyclable smart paper anticounterfeiting dynamic information storage. This work presents novel approach developing

Язык: Английский

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Bis-spirocyclic diol monomers and polyurethanes derived from citric acid: Synthesis, properties, electrospinnability, and evaluation of chemical recyclability

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 163525 - 163525

Опубликована: Май 1, 2025

Язык: Английский

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Controllable Modification of Rubber Achieved through Biobased Inverse Vulcanized Compounds

ACS Applied Polymer Materials, Год журнала: 2025, Номер unknown

Опубликована: Июнь 2, 2025

Язык: Английский

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Digital Light Processing 3D Printing of Isosorbide- and Vanillin-Based Ester and Ester–Imine Thermosets: Structure–Property Recyclability Relationships

ACS Sustainable Chemistry & Engineering, Год журнала: 2023, Номер 11(39), С. 14601 - 14613

Опубликована: Сен. 19, 2023

Four isosorbide-based photocurable resins were designed to reveal correlations between the composition and chemical structure, digital light processing (DLP) three-dimensional (3D) printability, thermoset properties, recyclability. Especially, role of functional groups, i.e., concentration ester groups vs combination imine functionalities, in recyclability was investigated. The consisted methacrylated isosorbide alone or with vanillin a flexible Schiff-base. significantly affected their 3D printability as well physical properties resulting thermosets. results indicated potential confer rigidity thermosets some negative effects on printing quality solvent-resistance properties. An increase resin enabled us overcome these drawbacks, leading, however, lower thermal stability. replacement Schiff-base decreased networks, ensuring, other hand, improved highlighted an almost complete preservation elastic modulus after reprocessing recycling ester-imine thermosets, thanks presence two distinct dynamic covalent bonds network; functions played significant success procedure.

Язык: Английский

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Isosorbide-Based Acrylic Pressure-Sensitive Adhesives Through UV-Cured Crosslinking with a Balance Between Adhesion and Cohesion

Polymers, Год журнала: 2024, Номер 16(22), С. 3178 - 3178

Опубликована: Ноя. 14, 2024

The development of sustainable pressure-sensitive adhesives (PSAs) from natural biomass resources has attracted increasing attention owing to their non-toxic, biocompatible, and biodegradable features. In this study, a bio-based acrylic PSA with tunable adhesion cohesion was synthesized by selective chemical modification isosorbide-5-acrylate (IA) its copolymerization butyl acrylate acid through UV-curing crosslinking. During the process, isosorbide diacrylate ester (IDAE) served as crosslinker, effectively improving crosslinking degree PSA. impact IA IDAE on mechanical properties studied. Moreover, achieve balance between cohesion, optimal composition identified. addition significantly enhances stiffness Furthermore, combined effect improves overall demonstrates peel force 13.9 N/25 mm persistent time 6820 min, promising replace traditional petroleum-based PSAs.

Язык: Английский

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Flame‐Retardant Self‐Healing Polymers: A Review

Journal of Polymer Science, Год журнала: 2024, Номер unknown

Опубликована: Дек. 25, 2024

ABSTRACT Developing multifunctional flame retardants (FRs) has become a strategy to reply on needs for advanced polymers. Self‐healing polymers are an emerging class of polymeric materials, which have been upgraded progressively, and recently taken the advantage fire safety. Correspondingly, diverse industries like aerospace, automotive, construction consumer electronics benefited from flame‐retardant self‐healing underlines their increasing contribution modern technologies. The characteristics stem intricate chemical physical interactions, adopting self‐directed repair mechanisms leading eliminating need frequent replacements, subsequently lowering maintenance costs environmental impact. This review summarizes advantages with emphasis exploring highly innovative advancements among bio‐based hydrogels, aerogels, coatings, thin films, lithium‐ion batteries ionotronic skin (‐i‐skin) structures embedding sensing features smoke detection exposure warnings, further broadening application in smart technologies safety‐critical infrastructure. outcomes reports outline challenges remaining developing such multifaceted materials view lack information due limited or exclusive investigations. However, research may facilitate dehydration, thermal shielding, free radical quenching contributing retardancy performance Sustainability circular economy requirements briefly discussed, addition outlining remarks future developments.

Язык: Английский

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