The high specific surface area of multilayered two-dimensional carbides called MXenes, is a critical feature for their use in energy storage systems, especially supercapacitors. Therefore, the possibility of controlling this parameter is highly desired. This work presents the results of the influence of oxygen concentration during Ti3AlC2 ternary carbide—MAX phase preparation on α-Al2O3 particles content, and thus the porosity and specific surface area of the Ti3C2Tx MXenes. In this research, three different Ti3AlC2 samples were prepared, based on TiC-Ti2AlC powder mixtures, which were conditioned and cold pressed in argon, air and oxygen filled glove-boxes. As-prepared pellets were sintered, ground, sieved and etched using hydrofluoric acid. The MAX phase and MXene samples were analyzed using scanning electron microscopy and X-ray diffraction. The influence of the oxygen concentration on the MXene structures was confirmed by Brunauer-Emmett-Teller surface area determination. It was found that oxygen concentration plays an important role in the formation of α-Al2O3 inclusions between MAX phase layers. The mortar grinding of the MAX phase powder and subsequent MXene fabrication process released the α-Al2O3 impurities, which led to the formation of the porous MXene structures. However, some non-porous α-Al2O3 particles remained inside the MXene structures. Those particles were found ingrown and irremovable, and thus decreased the MXene specific surface area.
A nitrogen-superdoped graphene with diamond-like interlayer bonds is obtained via the radical chemistry of fluorographene, affording a symmetric supercapacitor with an energy density of 200 W h L−1 at a power of 2.6 kW L−1 and 143 W h L−1 at 52 kW L−1.
Owing
to its high surface area and excellent conductivity, graphene
is considered an efficient electrode material for supercapacitors.
However, its restacking in electrolytes hampers its broader utilization
in this field. Covalent graphene functionalization is a promising
strategy for providing more efficient electrode materials. The chemistry
of fluorographene is particularly attractive as it allows scalable
chemical production of useful graphene derivatives. Nevertheless,
the influence of chemical composition on the capacitance of graphene
derivatives is a largely unexplored field in nanomaterials science,
limiting further development of efficient graphene-based electrode
materials. In the present study, we obtained well-defined graphene
derivatives differing in chemical composition but with similar morphologies
by controlling the reaction time of 5-aminoisophthalic acid with fluorographene.
The gravimetric specific capacitance ranged from 271 to 391 F g
–1
(in 1 M Na
2
SO
4
), with the maximum
value achieved by a delicate balance between the amount of covalently
grafted functional groups and density of the sp
2
carbon
network governing the conductivity of the material. Molecular dynamics
simulations showed that covalent grafting of functional groups with
charged and ionophilic/hydrophilic character significantly enhanced
the ionic concentration and hydration due to favorable electrostatic
interactions among the charged centers and ions/water molecules. Therefore,
conductive and hydrophilic graphitic surfaces are important features
of graphene-based supercapacitor electrode materials. These findings
provide important insights into the role of chemical composition on
capacitance and pave the way toward designing more efficient graphene-based
supercapacitor electrode materials.
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