| 1. |
- Ahmed, Heba, et al.
(author)
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Recovery of oxidized two-dimensional MXenes through high frequency nanoscale electromechanical vibration
- 2023
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In: Nature Communications. - : NATURE PORTFOLIO. - 2041-1723. ; 14:1
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Journal article (peer-reviewed)abstract
- MXenes hold immense potential given their superior electrical properties. The practical adoption of these promising materials is, however, severely constrained by their oxidative susceptibility, leading to significant performance deterioration and lifespan limitations. Attempts to preserve MXenes have been limited, and it has not been possible thus far to reverse the materials performance. In this work, we show that subjecting oxidized micron or nanometer thickness dry MXene films-even those constructed from nanometer-order solution-dispersed oxidized flakes-to just one minute of 10 MHz nanoscale electromechanical vibration leads to considerable removal of its surface oxide layer, whilst preserving its structure and characteristics. Importantly, electrochemical performance is recovered close to that of their original state: the pseudocapacitance, which decreased by almost 50% due to its oxidation, reverses to approximately 98% of its original value, with good capacitance retention ( approximate to 93%) following 10,000 charge-discharge cycles at 10 A g(-1). These promising results allude to the exciting possibility for rejuvenating the material for reuse, therefore offering a more economical and sustainable route that improves its potential for practical translation. Despite their vast potential, the practical deployment of MXenes has been hampered by their tendency to be oxidized. Here, the authors show that simply vibrating MXene films in just a minute can remove the oxide layer formed and restore their electrochemical performance close to its original state.
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| 2. |
- Ahmed, Heba, et al.
(author)
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Ultrafast assembly of swordlike Cu-3(1,3,5-benzenetricarboxylate)(n) metal-organic framework crystals with exposed active metal sites
- 2020
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In: Nanoscale Horizons. - : ROYAL SOC CHEMISTRY. - 2055-6764 .- 2055-6756. ; 5:7, s. 1050-1057
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Journal article (peer-reviewed)abstract
- Owing to their large surface area and high uptake capacity, metal-organic frameworks (MOFs) have attracted considerable attention as potential materials for gas storage, energy conversion, and electrocatalysis. Various strategies have recently been proposed to manipulate the MOF surface chemistry to facilitate exposure of the embedded metal centers at the crystal surface to allow more effective binding of target molecules to these active sites. Nevertheless, such strategies remain complex, often requiring strict control over the synthesis conditions to avoid blocking pore access, reduction in crystal quality, or even collapse of the entire crystal structure. In this work, we exploit the hydrodynamics and capillary resonance associated with acoustically-driven dynamically spreading and nebulizing thin films as a new method for ultrafast synthesis of swordlike Cu-3(1,3,5-benzenetricarboxylate)(n) (Cu-BTC) MOFs with unique monoclinic crystal structures (P2(1)/n) distinct to that obtained via conventional bulk solvothermal synthesis, with swordlike morphologies whose lengths far exceed their thicknesses. Through pulse modulation and taking advantage of the rapid solvent evaporation associated with the high nebulisation rates, we are also able to control the thicknesses of these large aspect ratio (width and length with respect to the thickness) crystals by arresting their vertical growth, which, in turn, allows exposure of the metal active sites at the crystal surface. An upshot of such active site exposure on the crystal surface is the concomitant enhancement in the conductivity of the MOF, evident from the improvement in its current density by two orders of magnitude.
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| 3. |
- Alijani, Hossein, et al.
(author)
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Acoustomicrofluidic Synthesis of Pristine Ultrathin Ti3C2Tz MXene Nanosheets and Quantum Dots
- 2021
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In: ACS Nano. - : AMER CHEMICAL SOC. - 1936-0851 .- 1936-086X. ; 15:7, s. 12099-12108
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Journal article (peer-reviewed)abstract
- The conversion of layered transition metal carbides and/or nitrides (MXenes) into zero-dimensional structures with thicknesses and lateral dimensions of a few nanometers allows these recently discovered materials with exceptional electronic properties to exploit the additional benefits of quantum confinement, edge effects, and large surface area. Conventional methods for the conversion of MXene nanosheets and quantum dots, however, involve extreme conditions such as high temperatures and/or harsh chemicals that, among other disadvantages, lead to significant degradation of the material as a consequence of their oxidation. Herein, we show that the large surface acceleration.on the order of 10 million gs.produced by high-frequency (10 MHz) nanometer-order electromechanical vibrations on a chipscale piezoelectric substrate is capable of efficiently nebulizing, and consequently dimensionally reducing, a suspension of multilayer Ti3C2Tz (MXene) into predominantly monolayer nanosheets and quantum dots while, importantly, preserving the material from any appreciable oxidation. As an example application, we show that the high-purity MXene quantum dots produced using this room-temperature chemical-free synthesis method exhibit superior performance as electrode materials for electrochemical sensing of hydrogen peroxide compared to the highly oxidized samples obtained through conventional hydrothermal synthesis. The ability to detect concentrations as low as 5 nM is a 10-fold improvement to the best reported performance of Ti3C2Tz MXene electrochemical sensors to date.
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| 4. |
- El Ghazaly, Ahmed, et al.
(author)
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Ultrafast, One-Step, Salt-Solution-Based Acoustic Synthesis of Ti3C2 MXene
- 2021
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In: ACS Nano. - : American Chemical Society (ACS). - 1936-0851 .- 1936-086X. ; 15:3, s. 4287-4293
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Journal article (peer-reviewed)abstract
- The current quest for two-dimensional transition metal carbides and nitrides (MXenes) has been to circumvent the slow, hazardous, and laborious multistep synthesis procedures associated with conventional chemical MAX phase exfoliation. Here, we demonstrate a one-step synthesis method with local Ti3AlC2 MAX to Ti3C2Tz MXene conversion on the order of milliseconds, facilitated by proton production through solution dissociation under megahertz frequency acoustic excitation. These protons combined with fluorine ions from LiF to selectively etch the MAX phase into MXene, whose delamination is aided by the acoustic forcing. These results have important implications for the future applicability of MXenes, which crucially depend on the development of more efficient synthesis procedures. For proof-of-concept, we show that flexible electrodes fabricated by this method exhibit comparable electrochemical performance to that previously reported.
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