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A conceptual change in crystallisation mechanisms of oxide materials from solutions in closed systems.

ABSTRACT: Atomic and molecular level interactions in solutions dictate the structural and functional attributes of crystals. These features clearly dictate the properties of materials and their applicability in technologies. However, the microscopic phenomena of particle formation-nucleation and growth-in real systems are still not fully understood. Specifically, crystallisation occurring in closed systems are largely unproven. Combining coherent experimental data, we here demonstrate a fundamental nucleation-growth mechanism that occurs in a model zinc oxide system when particles are formed under continuous, rapid heating under closed reaction conditions. Defying all previous reports, we show that the nucleation commences only when the heating is terminated. A prenucleation clusters pathway is observed for nucleation, followed by crystallite assembly-growth. We show that the nucleation-growth processes result from temporal and dynamic activity of constituent ions and gaseous molecules in solution and by the irreversible expulsion of the dissolved gaseous molecules. We suggest that this nucleation process is generic to most closed systems that go through precipitation, and, therefore, important for the crystallisation of a variety of metal oxides, composites and minerals. We anticipate that the work may be a platform for future experimental and theoretical investigation promoting deeper understanding of the nucleation-growth phenomena of a variety of practical systems.

SUBMITTER: Padmanabhan SC

PROVIDER: S-EPMC7592049 | biostudies-literature | 2020 Oct

REPOSITORIES: biostudies-literature

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A conceptual change in crystallisation mechanisms of oxide materials from solutions in closed systems.

Padmanabhan Sibu C SC Collins Timothy W TW Pillai Suresh C SC McCormack Declan E DE Kelly John M JM Holmes Justin D JD Morris Michael A MA

Scientific reports 20201027 1

Atomic and molecular level interactions in solutions dictate the structural and functional attributes of crystals. These features clearly dictate the properties of materials and their applicability in technologies. However, the microscopic phenomena of particle formation-nucleation and growth-in real systems are still not fully understood. Specifically, crystallisation occurring in closed systems are largely unproven. Combining coherent experimental data, we here demonstrate a fundamental nuclea ...[more]

PMID: 33110206

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Project description:Phase change materials (PCMs) in the form of fibers or fibrous mats with exceptional thermal energy storage ability and tunable working temperature are of high interest to produce smart thermoregulating textiles, useful for increasing human thermal comfort while avoiding energy waste. Common organic PCMs suffer from instability in their molten state, which limits their applicability as highly performing fibrous systems. In this work, electrospun fibrous mats made of polyethylene oxide (PEO), a PCM with excellent thermal properties and biocompatibility, were fabricated and their shape instability in the molten state was improved through UV photo-crosslinking. The characterization aimed to assess the performance of these shape-stable electrospun mats as nanofibrous PCMs for thermal management applications. In addition to an enhanced resistance to water-based solvents, UV-cured electrospun PEO mats demonstrated a remarkable latent heat (≈112 J/g), maintained over 80 heating/cooling cycles across the phase change temperature. Moreover, their morphological stability above their melting point was demonstrated both macroscopically and microscopically, with the retention of the initial nanofibrous morphology. Tensile mechanical tests demonstrated that the UV crosslinking considerably enhanced the ultimate properties of the fibrous mat, with a five-fold increase in both the tensile strength (from 0.15 MPa to 0.74 MPa) and the strain at break (from 2.5% to 12.2%) compared to the uncrosslinked mat. In conclusion, the photo-crosslinked electrospun PEO material exhibited high thermal properties and good shape stability without displaying leakage; accordingly, in the proposed PCM system, the necessity for encapsulation or use of a supporting layer has been eliminated. Photo-crosslinking thus proved itself as an effective, fast, and environmentally friendly method to dramatically improve the shape-stability of nanofibrous PEO electrospun mats for smart thermoregulating textiles.

Dataset Information

A conceptual change in crystallisation mechanisms of oxide materials from solutions in closed systems.

Publications

A conceptual change in crystallisation mechanisms of oxide materials from solutions in closed systems.

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