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Abstract MXenes, a new class of 2D transition metal carbides, nitrides, and carbonitrides, have attracted much attention due to their outstanding properties. Here, we report the broadband spatial self‐phase modulation of Ti2CTxMXene nanosheets dispersed in deionized water in the visible to near‐infrared regime, highlighting the broadband nonlinear optical (NLO) response of Ti2CTxMXene. Using ultrafast pulsed laser excitation, the nonlinear refractive indexn2and the third‐order nonlinear susceptibilityof Ti2CTxMXene were measured to be ∼10−13m2/W and ∼ 10−10esu, respectively. Leveraging the large optical nonlinearity of Ti2CTxMXene, an all‐optical modulator in the visible regime was fabricated based on the spatial cross‐phase modulation effect. This work suggests that 2D MXenes are ideal broadband NLO materials with excellent prospects in NLO applications. image
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This content will become publicly available on February 14, 2026
Record Efficiency of β‐Phase PVDF‐MXene Composites in Thin‐Film Dielectric Capacitors
Abstract Polyvinylidene fluoride (PVDF) is a semicrystalline polymer used in thin‐film dielectric capacitors because of its inherently high dielectric constant and low loss tangent. Its dielectric constant can be increased by the formation and alignment of its β‐phase crystalline structure, which can be facilitated by 2D nanofillers. 2D carbides and nitrides, MXenes, are promising candidates due to their notable dielectric permittivity and ability to increase interfacial polarization. Still, their mixing is challenging due to weak interfacial interactions and poor dispersibility of MXenes in PVDF. This work explores a novel method for delaminating Ti3C2TxMXene directly into organic solvents while maintaining flake size and quality, as well as the use of a non‐solvent‐induced phase separation method for producing both dense and porous PVDF‐MXene composite films. A deeper understanding of dielectric behavior in these composites is reached by examining MXenes with both mixed and pure chlorine terminations in PVDF matrices. Thin‐film capacitors fabricated from these composites display ultrahigh discharge energy density, exceeding 45 J cm−3with 95% efficiency. The PVDF‐MXene composites are also processed using a green and sustainable solvent, propylene carbonate.
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- PAR ID:
- 10571882
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 37
- Issue:
- 12
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract The origin of MXene's excellent electromagnetic shielding performance is not fully understood. MXene films, despite being inhomogeneous at the nanometer scale, are often treated as if they are compared to bulk conductors. It is reasonable to wonder if the treatment of MXene as a homogeneous material remains valid at very small film thickness and if it depends on the interlayer spacing. The goal of the present work is to test if the homogeneous material model is applicable to nanometer‐thin Ti3C2TxMXene films and, if so, to investigate how the model parameters may depend on variations in MXene interlayer spacings. MXene films containing flakes with interlayer spacing between 1.9 and 5.5 Å have been prepared using various intercalating agents. It is shown that modeling the films as being homogeneous agrees with experimental tests in the microwave frequency range. Microwave conductivity and dielectric constant parameters are estimated for the homogeneous film model by fitting measured results. The direct current (DC) conductivity matches the estimated microwave conductivity on the order of magnitude. A highly effective dielectric constant provides a good fit for the lower conductivity MXene films. Optical absorption agrees with the homogeneous material model of thin films as well.more » « less
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Abstract MXenes are a new family of two-dimensional carbides and/or nitrides. Their 2D surfaces are typically terminated by O, OH and/or F atoms. Here we show that Ti3C2Tx—the most studied compound of the MXene family—is a good acid catalyst, thanks to the surface acid functionalities. We demonstrate this by applying Ti3C2Txin the epoxide ring-opening reaction of styrene oxide (SO) and its isomerization in the liquid phase. Modifying the MXene surface changes the catalytic activity and selectivity. By oxidizing the surface, we succeeded in controlling the type and number of acid sites and thereby improving the yield of the mono-alkylated product to >80%. Characterisation studies show that a thin oxide layer, which forms directly on the Ti3C2Txsurface, is essential for catalysing the SO ring-opening. We hypothesize that two kinds of acid sites are responsible for this catalysis: In the MXene, strong acid sites (both Lewis and Brønsted) catalyse both the ring-opening and the isomerization reactions, while in the Mxene–TiO2composite weaker acid sites catalyse only the ring-opening reaction, increasing the selectivity to the mono-alkylated product.more » « less
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Abstract Surface chemistry and core composition of 2D MXenes play a major role in their interfacial properties, but the determination and quantification of their bonding environments remain challenging. X‐ray Photoelectron Spectroscopy (XPS) is a method of choice that is broadly utilized but is often hindered by large uncertainties and systematic bias due to adsorbed species such as adventitious carbon or etching residues. In this work, energy‐dependent XPS and depth profile modeling of the Ti3C2TxMXene surface are employed to differentiate the contributions from the MXene and the adsorbed species, thereby increasing the accuracy of quantification. In comparison, uncorrected lab‐based XPS suffers from a systematic overestimation of Ti vacancies by 7% and an underestimation of terminal atoms, particularly F, by as much as 15%. Interestingly, it is found that a simple inelastic mean free path correction is sufficient to address the issue and reveals extremely low defects in Ti3C2TxMXene synthesized using the HF/HCl etching route. Soft X‐ray Absorption Spectroscopy (XAS), supported by Density Functional Theory (DFT) calculations, also demonstrates a high chemical sensitivity of the surface terminations. This work provides novel insights into XPS quantification and the use of XAS for probing the carbide core and surface chemistry of Ti3C2TxMXenes.more » « less
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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.more » « less
