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Polycaprolactone Adsorption and Nucleation onto Graphite Nanoplates for Highly Flexible, Thermally Conductive, and Thermomechanically Stiff Nanopapers.

ABSTRACT: Free-standing nanopapers based on graphene and its related materials have been widely studied and proposed for flexible heat spreader applications. Given that these materials are typically brittle, this work reports the exploitation of polycaprolactone (PCL) as a polymer binder to enhance resistance and flexibility of nanopapers based on graphite nanoplates (GNP), while maintaining a high thermal conductivity. Properties of nanopapers appear to correlate with the excellent PCL adhesion and strong nucleation of the surface of GNP flakes. Furthermore, different crystalline populations were observed for PCL within the nanopaper and were investigated in detail via differential scanning calorimetry advanced techniques and X-ray diffraction. These demonstrated the coexistence of conventional unoriented PCL crystals, oriented PCL crystals obtained as a consequence of the strong nucleation effect, and highly stable PCL fractions explained by the formation of crystalline pre-freezing layers, the latter having melting temperatures well above the equilibrium melting temperature for pristine PCL. This peculiar crystallization behavior of PCL, reported in this paper for the first time for a tridimensional structure, has a direct impact on material properties. Indeed, the presence of high thermal stability crystals, strongly bound to GNP flakes, coexisting with the highly flexible amorphous fraction, delivers an ideal solution for the strengthening and toughening of GNP nanopapers. Thermomechanical properties of PCL/GNP nanopapers, investigated both on a heating ramp and by creep tests at high temperatures, demonstrated superior stiffness well above the conventional melting temperature of PCL. At the same time, a thermal conductivity > 150 W/m·K was obtained for PCL/GNP nanopapers, representing a viable alternative to traditional metals in terms of heat dissipation, while affording flexibility and light weight, unmatched by conventional thermally conductive metals or ceramics. Besides the obtained performance, the formation of polymer crystals that are stable above the equilibrium melting temperature constitutes a novel approach in the self-assembly of highly ordered nanostructures based on graphene and related materials.

SUBMITTER: Li K

PROVIDER: S-EPMC8678991 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:The adsorption of thallium (Tl) onto phyllosilicate minerals plays a critical role in the retention of Tl in soils and sediments and the potential transfer of Tl into plants and groundwater. Especially micaceous minerals are thought to strongly bind monovalent Tl(I), in analogy to their strong binding of Cs. To advance the understanding of Tl(I) adsorption onto phyllosilicate minerals, we studied the adsorption of Tl(I) onto Na- and K-saturated illite and Na-saturated smectite, two muscovites, two vermiculites and a naturally Tl-enriched soil clay mineral fraction. Macroscopic adsorption isotherms were combined with the characterization of the adsorbed Tl by X-ray absorption spectroscopy (XAS). In combination, the results suggest that the adsorption of Tl(I) onto phyllosilicate minerals can be interpreted in terms of three major uptake paths: (i) highest-affinity inner-sphere adsorption of dehydrated Tl+ on a very low number of adsorption sites at the wedge of frayed particle edges of illite and around collapsed zones in vermiculite interlayers through complexation between two siloxane cavities, (ii) intermediate-affinity inner-sphere adsorption of partially dehydrated Tl+ on the planar surfaces of illite and muscovite through complexation onto siloxane cavities, (iii) low-affinity adsorption of hydrated Tl+, especially in the hydrated interlayers of smectite and expanded vermiculite. At the frayed edges of illite particles and in the vermiculite interlayer, Tl uptake can lead to the formation of new wedge sites that enable further adsorption of dehydrated Tl+. On the soil clay fraction, a shift in Tl(I) uptake from frayed edge sites (on illite) to planar sites (on illite and muscovite) was observed with increasing Tl(I) loading. The results from this study show that the adsorption of Tl(I) onto phyllosilicate minerals follows the same trends as reported for Cs and Rb and thus suggests that concepts to describe the retention of (radio)cesium by different types of phyllosilicate minerals in soils, sediments and rocks are also applicable to Tl(I).

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Polycaprolactone Adsorption and Nucleation onto Graphite Nanoplates for Highly Flexible, Thermally Conductive, and Thermomechanically Stiff Nanopapers.

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