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Abstract Ti3C2Tx(MXenes) are novel 2D nanomaterials with exceptional electrical conductivity. Their surfaces are covered with functional groups that may significantly affect material properties such as hydrophobicity, electrical conductivity, and oxidation resistance. The role of these terminations in high-temperature ceramic systems with regard to phase and microstructural evolution has not been investigated. In this study, Ti3C2Tx-SiOC 2D nanocomposites were fabricated with -F and -OH terminated MXene to evaluate the role of surface terminations in silane coupling and phase formation during the polymer-to-ceramic transformation. X-ray diffraction (XRD), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), and X-ray photoelectron spectroscopy (XPS) identified self-etching mechanisms caused by F-terminated Ti3C2Txand revealed that the F surface terminations were retained in the MXene structure until evolution at ~ 550 °C. Evolved F reacted with Si–H bonds in the transforming ceramic matrix, causing additional mass loss and volumetric deformation. LiOH alkalization was shown to suppress the self-etching phenomenon through the substitution of F groups with OH on the nanosheet surface. Furthermore, F terminations were determined to only engage in hydrogen bonding with silane molecules as opposed to covalent linkages with OH terminations, which accelerated silane removal and Ti3C2Txdegradation. The study provides a fundamental understanding of the nature and behavior of MXene surface terminations in the context of high-temperature ceramic nanocomposite fabrication.
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Bioencapsulated MXene Flakes for Enhanced Stability and Composite Precursors
Abstract Here it is shown that Ti3C2TxMXene flakes can be co‐assembled with recombinant silk fibroin in aqueous suspensions with silk fibroin nanolayers uniformly covering individual flakes. These bioencapsulated flakes evolve with time due to the gradual growth of silk bundles having β‐sheet secondary organization with unique nanofibrillar morphologies extending across flake edges and forming long fringes around individual MXene flakes. This spontaneous reorganization of recombinant silk suggests surface template‐initiated formation of intramolecular hydrogen bonding of silk backbones assisted by intermolecular electrostatic and hydrogen bonding with the MXene flake. The formation of dense and hydrophobic β‐sheets results in development of a protective shell that hinders the surface oxidation of Ti3C2Txin colloidal solution in water and significantly extends the storage life of the individual MXene flakes. Moreover, assembly into organized laminated composites with individual bioencapsulated flakes tightly interconnected via biopolymer bundles and hairs produces robust freestanding electrically conductive membranes with enhanced transport properties.
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- Award ID(s):
- 1740795
- PAR ID:
- 10455652
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Functional Materials
- Volume:
- 30
- Issue:
- 43
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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