- Award ID(s):
- NSF-PAR ID:
- Date Published:
- Journal Name:
- 2D Materials
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract High electrical conductivity is desired in MXene films for applications such as electromagnetic interference shielding, antennas, and electrodes for electrochemical energy storage and conversion applications. Due to the acid etching-based synthesis method, it is challenging to deconvolute the relative importance that factors such as chemical composition and flake size contribute to resistivity. To understand the intrinsic and extrinsic contributions to the macroscopic electronic transport properties, a systematic study controlling compositional and structural parameters was conducted with eight solid solutions in the Ti y Nb 2− y CT x system. In particular, we investigated the different roles played by metal (M)-site composition, flake size, and d -spacing on macroscopic transport. Hard x-ray photoemission spectroscopy and spectroscopic ellipsometry revealed changes to electronic structure induced by the M-site alloying. Consistent with the spectroscopic results, the low- and room-temperature conductivities and effective carrier mobility are correlated with the Ti content, while the impact of flake size and d -spacing is most prominent in low-temperature transport. The results provide guidance for designing and engineering MXenes with a wide range of conductivities.more » « less
Abstract 2D material hydrogels have recently sparked tremendous interest owing to their potential in diverse applications. However, research on the emerging 2D MXene hydrogels is still in its infancy. Herein, we show a universal 4D printing technology for manufacturing MXene hydrogels with customizable geometries, which suits a family of MXenes such as Nb 2 CT x , Ti 3 C 2 T x , and Mo 2 Ti 2 C 3 T x . The obtained MXene hydrogels offer 3D porous architectures, large specific surface areas, high electrical conductivities, and satisfying mechanical properties. Consequently, ultrahigh capacitance (3.32 F cm −2 (10 mV s −1 ) and 233 F g −1 (10 V s −1 )) and mass loading/thickness-independent rate capabilities are achieved. The further 4D-printed Ti 3 C 2 T x hydrogel micro-supercapacitors showcase great low-temperature tolerance (down to –20 °C) and deliver high energy and power densities up to 93 μWh cm −2 and 7 mW cm −2 , respectively, surpassing most state-of-the-art devices. This work brings new insights into MXene hydrogel manufacturing and expands the range of their potential applications.more » « less
Transition metal carbides (MXenes) are an emerging family of highly conductive two-dimensional materials with additional functional properties introduced by surface terminations. Further modification of the surface terminations makes MXenes even more appealing for practical applications. Herein, we report a facile and environmentally benign synthesis of reduced Ti 3 C 2 T x MXene (r-Ti 3 C 2 T x ) via a simple treatment with l -ascorbic acid at room temperature. r-Ti 3 C 2 T x shows a six-fold increase in electrical conductivity, from 471 ± 49 for regular Ti 3 C 2 T x to 2819 ± 306 S m −1 for the reduced version. Additionally, we show an enhanced oxidation stability of r-Ti 3 C 2 T x as compared to regular Ti 3 C 2 T x . An examination of the surface-enhanced Raman scattering (SERS) activity reveals that the SERS enhancement factor of r-Ti 3 C 2 T x is an order of magnitude higher than that of regular Ti 3 C 2 T x . The improved SERS activity of r-Ti 3 C 2 T x is attributed to the charge transfer interaction between the MXene surface and probe molecules, re-enforced by an increased electronic density of states (DOS) at the Fermi level of r-Ti 3 C 2 T x . The findings of this study suggest that reduced MXene could be a superior choice over regular MXene, especially for the applications that employ high electronic conductivity, such as electrode materials for batteries and supercapacitors, photodetectors, and SERS-based sensors.more » « less
MXenes, a family of 2D transition‐metal carbides and nitrides, have excellent electrical conductivity and unique optical properties. However, MXenes oxidize in ambient conditions, which is accelerated upon heating. Intercalation of water also causes hydrolysis accelerating oxidation. Developing new tools to readily characterize MXenes’ thermal stability can enable deeper insights into their structure–property relationships. Here, in situ spectroscopic ellipsometry (SE) is employed to characterize the optical properties of three types of MXenes (Ti3C2T
x, Mo2TiC2T x, and Ti2CT x) with varied composition and atomistic structures to investigate their thermal degradation upon heating under ambient environment. It is demonstrated that changes in MXene extinction and optical conductivity in the visible and near‐IR regions correlate well with the amount of intercalated water and hydroxyl termination groups and the degree of oxidation, measured using thermogravimetric analysis. Among the three MXenes, Ti3C2T xand Ti2CT x, respectively, have the highest and lowest thermal stability, indicating the role of transition‐metal type, synthesis route, and the number of atomic layers in MXene flakes. These findings demonstrate the utility of SE as a powerful in situ technique for rapid structure–property relationship studies paving the way for the further design, fabrication, and property optimization of novel MXene materials.
2D carbides and nitrides (MXenes) are widely recognized for their exceptional promise for numerous applications. However, physical property measurements of their individual monolayers remain very limited despite their importance for revealing the intrinsic physical properties of MXenes. The first mechanical and electrical measurements of individual single‐layer flakes of Nb4C3T
xMXene, which are prepared via an improved synthetic method are reported. Characterization of field‐effect transistor devices based on individual single‐layer Nb4C3T xflakes shows an electrical conductivity of 1024 ± 165 S cm−1, which is two orders of magnitude higher than the previously reported values for bulk Nb4C3T xassemblies, and an electron mobility of 0.41 ± 0.27 cm2V−1s−1. Atomic force microscopy nanoindentation measurements of monolayer Nb4C3T xmembranes yield an effective Young's modulus of 386 ± 13 GPa, assuming a membrane thickness of 1.26 nm. This is the highest value reported for nanoindentation measurements of solution‐processable 2D materials, revealing the potential of Nb4C3T xas a primary component for various mechanical applications. Finally, the agreement between the mechanical properties of 2D Nb4C3T xMXene and cubic NbC suggests that the extensive experimental data on bulk carbides could be useful for identifying new MXenes with improved functional characteristics.