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  1. Abstract

    Driving the pseudocapacitive redox intercalation in 2DMXenes with neutral electrolytes is important for safer, more sustainable, and improved electrochemical charge storage. Single transition metal MXenes, such as Ti3C2, have shown great promise for energy storage, owing to their high conductivity and redox activity. Mixed metallic MXenes, such as out‐of‐plane ordered Mo2Ti2C3, have remained underexplored in energy storage because of the absence of redox activity in most of the electrolytes. Simultaneous structural modifications and instigating intercalation pseudocapacitance in neutral electrolytes could be a viable strategy for enhancing their electrochemical properties. Herein, a facile synthesis of partially oxidized Mo2Ti2C3MXene (PO‐Mo2Ti2C3) exhibiting improved charge storage capability is demonstrated. Optical, structural, and spectroscopic analyses indicate the formation of oxide nanostructures upon thermal oxidation of Mo2Ti2C3. This leads to an enhanced energy storage capability with remarkably improved cyclability as well as a high Coulombic efficiency in a neutral LiCl electrolyte. This work highlights the importance of structural modifications of MXenes to enhance their charge storage and shows the promise of less explored double transition metal MXenes in energy storage.

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  3. Abstract

    MXenes constitute a rapidly growing family of 2D materials that are promising for optoelectronic applications because of numerous attractive properties, including high electrical conductivity. However, the most widely used titanium carbide (Ti3C2Tx) MXene transparent conductive electrode exhibits insufficient environmental stability and work function (WF), which impede practical applications Ti3C2Txelectrodes in solution‐processed optoelectronics. Herein, Ti3C2TxMXene film with a compact structure and a perfluorosulfonic acid (PFSA) barrier layer is presented as a promising electrode for organic light‐emitting diodes (OLEDs). The electrode shows excellent environmental stability, highWFof 5.84 eV, and low sheet resistanceRSof 97.4 Ω sq−1. The compact Ti3C2Txstructure after thermal annealing resists intercalation of moisture and environmental contaminants. In addition, the PFSA surface modification passivates interflake defects and modulates theWF. Thus, changes in theWFandRSare negligible even after 22 days of exposure to ambient air. The Ti3C2TxMXene is applied for large‐area, 10 × 10 passive matrix flexible OLEDs on substrates measuring 6 × 6 cm. This work provides a simple but efficient strategy to overcome both the limited environmental stability and lowWFof MXene electrodes for solution‐processable optoelectronics.

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  4. Abstract

    MXenes, two‐dimensional (2D) transition metal carbides and/or nitrides, possess surface termination groups such as hydroxyl, oxygen, and fluorine, which are available for surface functionalization. Their surface chemistry is critical in many applications. This article reports amine functionalization of Ti3C2TxMXene surface with [3‐(2‐aminoethylamino)‐propyl]trimethoxysilane (AEAPTMS). Characterization techniques such as X‐ray photoelectron spectroscopy verify the success of the surface functionalization and confirm that the silane coupling agent bonds to Ti3C2Txsurface both physically and chemically. The functionalization changes the MXene surface charge from −35 to +25 mV at neutral pH, which allows for in situ preparation of self‐assembled films. Further, surface charge measurements of the functionalized MXene at different pH values show that the functionalized MXene has an isoelectric point at a pH around 10.7, and the highest reported positive surface charge of +62 mV at a pH of 2.58. Furthermore, the existence of a mixture of different orientations of AEAPTMS and the simultaneous presence of protonated and free amine groups on the surface of Ti3C2Txare demonstrated. The availability of free amine groups on the surface potentially permits the fabrication of crosslinked electrically conductive MXene/epoxy composites, dye adsorbents, high‐performance membranes, and drug carriers. Surface modifications of this type are applicable to many other MXenes.

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  6. Abstract

    The cycle life of rechargeable lithium (Li)‐metal batteries is mainly restrained by dendrites growth on the Li‐metal anode and fast depletion of the electrolyte. Here, we report on a stable Li‐metal anode enabled by interconnected two‐dimensional (2D) arrays of niobium nitride (NbN) nanocrystals as the Li host, which exhibits a high Coulombic efficiency (>99 %) after 500 cycles. Combining theoretical and experimental analysis, it is inferred that this performance is due to the intrinsic properties of interconnected 2D arrays of NbN nanocrystals, such as thermodynamic stability against Li‐metal, high Li affinity, fast Li+migration, and Li+transport through the porous 2D nanosheets. Coupled with a lithium nickel–manganese–cobalt oxide cathode, full Li‐metal batteries were built, which showed high cycling stability under practical conditions – high areal cathode loading ≥4 mAh cm−2, low negative/positive (N/P) capacity ratio of 3, and lean electrolyte weight to cathode capacity ratio of 3 g Ah−1. Our results indicate that transition metal nitrides with a rationally designed structure may alleviate the challenges of developing dendrite‐free Li‐metal anodes.

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