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A Review on Layered Mineral Nanosheets Intercalated With DOI: 10.1002/macp.201800142 Article type: Trend A Review on Layered Mineral Nanosheets Intercalated with Hydrophobic/Hydrophilic Polymers and their Applications Danial Sangian*, Sina Naficy*, Fariba Dehghani and Yusuke Yamauchi Dr. D. Sangian International Center for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan Email: [email protected] Dr. S. Naficy, F. Dehghani School of Chemical and Biomolecular Engineering, The University of Sydney, Sydney, NSW 2006, Australia Email: [email protected] Y. Yamauchi School of Chemical Engineering, The University of Queensland, Brisbane, QLD 4072, Australia This is the author manuscript accepted for publication and has undergone full peer review but has not been through the copyediting, typesetting, pagination and proofreading process, which may lead to differences between this version and the Version of Record. Please cite this article as doi: 10.1002/macp.201800142. This article is protected by copyright. All rights reserved. Keywords: 2D nanosheets, inorganic layered materials, intercalation, exfoliation, nano-actuators. Abstract Materials with layered structures at the nanoscale have lately drawn significant attention from engineers and scientists in the fields of physics, chemistry, and mathematics, due to the unique characteristics that originate from their hierarchical structure. The nano-sized free space between each two adjacent layers, so-called the interlayer space, is an attractive place that can be manipulated by incorporating different molecular species to generate novel physical and mechanical behaviors. This review highlights the latest studies and new important developments on possible methods of intercalating popular species such as hydrophobic and hydrophilic polymers into the interlayer spaces of layered materials. It also provides a description of intercalation processes as well as final applications for better understanding as it is believed to be an effective factor in utilizing these materials in research and industry. Finally, this review gives perspectives on the future applicants of inorganic layered materials filled with polymers with different hydrophilicity properties. 1. Introduction Nanomaterials are a growing class of materials with at least one discrete dimension in nanometer scale 1-6. The nanoscale dimensionality of nanomaterials results in new properties that are remarkably different to those at bulk scales 7, such as metallic electrical conductivity in carbon nanotubes, excellent thermal conductivity in boron nitride nanosheets, significantly lower melting temperature and red color in gold nanoparticles and higher solar absorption in photovoltaic cells 8-9. Based on their unique characteristics, nanomaterials have been proposed for numerous task-specific This article is protected by copyright. All rights reserved. applications such as cosmetics, intelligent textiles, smart food packaging, controlled drug and gene delivery, tissue engineering, and highly efficient catalysts 10-16. In nanoscale size, the proportion of atoms located on the surface area of a nanoparticle to the total volume of atoms constructing the nanoparticle is considerably high 17. This high exposure of functional groups and atoms to the environment, which does not exist in macro scales, appears to have a strong impact on the properties of nanomaterials. Various species, from small molecules to large macromolecules, can interact with the functional groups at the surface of nanoparticles. The nature of these interfacial interactions and the type of guest species play important roles in determining the bulk properties of the hybrid systems. However, there are few examples available in which the full characteristics of nanomaterials arisen from their nanoscale structure have been adequately realized. The dilemma here is that while nanomaterials on their own offer unique properties, the nanocomposites made by them do not inherit such characteristics. As such, the key point in creation of new systems based on nanomaterials is to develop methods of fabrication that are capable of translating the nanoscale structural, physical, chemical or biological specifications of nanomaterials from nanometer scale to macroscale 18-20. Nanomaterials are divided into three major groups based on their molecular structure (Figure 1). When only one dimension of the nanomaterials is within the nanometer range, the particles are layered and referred to as two-dimensional (2D) nanomaterials. The 2D nanomaterials are particularly of interest since they provide the highest exposure of atoms and functional groups per surface area. Graphene, hexagonal boron nitride (hBN), different transition metal chacolgenides (TMCs), MXenes and MAX phases belong to this category of nanomaterials 21. Because of their high aspect ratio in two dimensions, the 2D nanomaterials offer unique planar properties including excellent thermal conductivity 22, electrical conductivity 23, and charge carrier mobilities in their planes 24, as well as high mechanical flexibility, and high optical and UV adsorptions 25. 1D nanomaterials (e.g. carbon nanotubes and silver nanowires) have two dimensions in nanometer scale 26. Similarly, 0D nanomaterials, such as quantum dots, are discrete nanoparticles when all their three dimensions are limited to nanometer scale. These 0D nanomaterials are also referred to as “isodimensional” materials 27. Dimensionality of materials plays a pivotal role in determining the properties of nanomaterials: for instance, 0D fullerenes (clusters) 28, 1D nanotubes 29, 2D graphene 30-31 and 3D graphite 32 offer significantly different properties due to their different dimensionality. This article is protected by copyright. All rights reserved. In this review, we focus on 2D nanolayered minerals as the most abundant and cost-effective class of nanoparticles. In addition to their availability, 2D mineral nanoparticles can offer unique engineering properties such as high surface reactivity, high adsorption, versatile chemical structure, high chemical resistivity, and processabillity. They often bring significant reinforcements into various properties of virgin organic networks such as polymers after physical intercalation of long polymer chains. These reinforcements in polymer science can include high moduli, increased strength and heat resistance, decrease gas permeability and flammability and biodegradability enhancement. We acknowledge that several excellent reviews33-35 have already been published on layered mineral nanosheets intercalated with organic species, which have broadened the understanding of this area of science. Therefore, in this review we mostly focus on the hydrophilicity behavior and final applications of these materials. 2. 2D Nanolayered Minerals In the 2D nanolayered materials the constituting atoms are positioned in flat layers. These layers are piled on top of each other like sheets of paper and held together with Van der Waals, polar, or ionic bonds. Disconnecting the staked sheets from each other in the bulk materials to expose the planar surface of each individual particle was an infeasible task until new methods such as oxidation, ion intercalation/exchange, surface and passivation by solvents were developed 36-43. In all these techniques, the space between two individual layers, so called the “interlayer space”, is first expanded by subjecting the bulk material to a combination of certain ions and solvents. Through this process, ions and solvent molecules diffuse into the space between the layers causing the expansion of the interlayer space as a consequence of generated repulsion forces 44-47. For example, water and polar solvents are capable of expanding layered materials with polar interlayer interaction 48. Table 1 categorizes the common types of inorganic layered materials according to their interlayer expansion type and charge carrier. However, the expansion range achieved by these techniques is limited to few nanometers and is not suitable for applications where better access to the surface area of the nanomaterials is required 43, 49. In order to sufficiently increase the interlayer space, weakly connected individual layers can be further separated by rapidly cancelling the atomic attractive forces between the layers using exfoliation (delamination) methods, either chemically or mechanically (shear or ultrasonication) 46-48. The combination of these processes leads to full separation of planar nanosheets leaving them fully suspended in media (Figure 2). This article is protected by copyright. All rights reserved. The discovery of exfoliation methods in 1990′s opened up a new chapter in materials science and technology 39, 47, 50, considering that the properties that had been seen in stacked layered materials considerably differ from those of their exfoliated counterparts 43, 51. The immediate observation was that the exfoliation processes could amplify some of the pre-exiting properties of the bulk layered materials, such as electrical conductivity in graphene, magneto-optical effects in Co-Al layered 52-54 double hydroxide (LDH), and photocatalystic activity in MoS2 . As a result, single layers of manganese 55, cobalt 56, tantalum 57, ruthenium 58, titanium 59 oxides and many other perovskite type structures have been produced from the bulk materials. In these examples, protonation via chemical intercalators was used to cause electrostatic repulsion between layers and separate the metal
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