Nitrogen and sulfur co-doped vanadium carbide MXene for highly reversible lithium-ion storage

New two-dimensional niobium and vanadium carbides have been synthesized by selective etching, at room temperature, of Al from Nb2AlC and V2AlC, respectively. These new matrials are promising electrode materials for Li-ion batteries, demonstrating good capability to handle high charge-discharge rates. Reversible capacities of 170 and 260 mA·h·g(-1) at 1 C, and 110 and 125 mA·h·g(-1) at 10 C were obtained for Nb2C and V2C-based electrodes, respectively.

MXene/carbon composite electrodes with high loadings of MXene were prepared via electrospinning. These flexible and free-standing electrodes exhibit high areal capacitance relative to pure carbon nanofibers and MXene-coated fibers and textiles. Free-standing Ti 3 C 2 T x MXene/carbon nanofiber electrodes are prepared via electrospinning Ti 3 C 2 T x MXene flakes with polyacrylonitrile (PAN) and carbonizing the fiber networks. Using this simple fabrication method, delaminated MXene flakes are embedded within carbon nanofibers and these fiber mats are used as electrodes without binders or additives. Unlike coated electrodes, which may suffer from the active material delaminating from the substrate during folding or bending, composite electrodes are stable and durable. Previous attempts to incorporate Ti 3 C 2 T x MXene into electrospun fibers resulted in low mass loadings, ∼1 wt% Ti 3 C 2 T x MXene. In this work, MXene flakes are added into PAN solutions at a weight ratio of 2 : 1 (MXene : PAN) in the spinning dope, producing fiber mats with up to 35 wt% MXene. Composite electrodes have high areal capacitance, up to 205 mF cm −2 at 50 mV s −1 , almost three times that of pure carbonized PAN nanofibers (70 mF cm −2 at 50 mV s −1 ). Compared with electrospun nanofibers spray-coated with Ti 3 C 2 T x , these composite fibers exhibit double the areal capacitance at 10 mV s −1 . This method can be used to produce MXene composite fibers using a variety of polymers, which have potential applications beyond energy storage, including filtration, adsorption, and electrocatalysis, where fibers with high aspect ratio, accessible surface, and porosity are desirable.

Abstract MXene films are attractive for advanced supercapacitor electrodes requiring high volumetric energy density due to their high redox capacitance combined with extremely high packing density. However, the self‐restacking of MXene flakes unavoidably decreases the volumetric performance, mass loading, and rate capability. Herein, a simple strategy is developed to prepare a flexible and free‐standing modified MXene/holey graphene film by filtration of the alkalized MXene and holey graphene oxide dispersions, followed by a mild annealing treatment. After terminal groups (—F/—OH) are removed, the increased proportion of Ti atoms enables more pseudocapacitive reaction. Meanwhile, the embedded holey graphene effectively prevents the self‐restacking of MXene and forms a high nanopore connectivity network, which is able to immensely accelerate the ion transport and shorten transport pathways for both ion and electron. When applied as electrode materials for supercapacitors, it can deliver an ultrahigh volumetric capacitance (1445 F cm−3) at 2 mV s−1, excellent rate capability, and high mass loading. In addition, the assembled symmetric supercapacitor demonstrates a fantastic volumetric energy density (38.6 Wh L−1), which is the highest value reported for MXene‐based electrodes in aqueous electrolytes. This work opens a new avenue for the further exploration of MXene materials in energy storage devices.