Ultrathin MXene Research Articles

Self-Assembled Ti3C2TX MXene Thin Films for High-Performance Ammonia Sensors

MXenes have emerged as a fascinating material for RT gas-sensing applications due to their outstanding properties. This work reports the design and fabrication of a high-performance ammonia sensor based on MXenes material. To improve its sensing performance, a MXenes nanosheets thin film with a thickness of ≈ 10 nm was prepared using a scalable self-assembled method. Specifically, we employed the controlled and enhanced interfacial self-assembled method to fabricate a continuous and conductive MXene ultra-thin film. The morphology and the structure of the produced MXene materials and their films were characterized by combining multi-characterization tools. Altoghether, these highlight the uniform and continuous deposition of the MXene nanosheets film on the glass substrate. The electrical characterization indicates a sheet resistance value of 4.82 × 105 Ω/sq. The fabricated devices present good RT sensing performances for NH3 detection, ranging from 1 to 20 ppm. This demonstrates the outstanding sensitivity of MXene with a value of 1.92 % for the lowest concentration (1 ppm), a fast response (179 s) and a recovery time of (612 s), which is related to the high quality of the ultra-thin MXene sensiting layer. Moreover, the sensors demonstrate high degree of stability and excellent reproducibility, make them suitable candidate for practical applications like environmental monitoring.

Design and Performance of Ultrathin MXene Nano-Absorber for Visible and Infrared Spectra

Design and Performance of Ultrathin MXene Nano-Absorber for Visible and Infrared Spectra

A unique three-dimensional network double-core–shell structure S@MnO2@MXene suppresses the shuttle effect in high-sulfur-content high-performance lithium-sulfur batteries

Lithium-sulfur (Li-S) batteries represent the most promising next-generation energy storage systems because of their high theoretical specific capacity and energy density. However, the severe shuttle effect and volume expansion of sulfur cathodes have impeded their commercial viability. Hence, accelerating the conversion of lithium polysulfides (LiPSs) is crucial for achieving efficient Li-S batteries. In this study, we employ a straightforward electrostatic self-assembly method to coat ultra-thin MXene nanosheets onto a S@MnO2 core–shell structure, resulting in a highly conductive three-dimensional network. This unique structure not only suppresses the diffusion of LiPSs but also accelerates electron and ion transfer, ensuring a rapid and efficient conversion of LiPSs. The CV curves of symmetrical cells and the Li2S deposition curves demonstrate a significant improvement in the catalytic performance of batteries with S@MnO2@MXene. The capacity of Li-S batteries achieved an impressive 842 mAh/g at the current density of 1C, with a minimal capacity decay of only 0.84 mAh/g per cycle within 500 cycles. Additionally, increasing the sulfur loading mass to 5.88 mg cm−2 resulted in an areal capacity of 6.33 mAh cm−2, demonstrating practical application potential.

Centrifugal-Gravity-Enforced Deposition of MXene Electrodes for High-Performance and Ultrastable Microsupercapacitors.

Two-dimensional (2D) transition metal carbides, known as MXenes, have captured much attention for their excellent electrical conductivity and electrochemical capability. However, the susceptibility of MXenes to oxidation, particularly Ti3C2Tx transforming into titanium dioxide upon exposure to ambient air, hinders their utilization for extended operational life cycles. This work introduces a simple and straightforward method for producing ultrathin MXene electrode films tailored for energy storage applications, employing centrifugal-gravity force. Our approach significantly suppresses the oxidation phenomenon that arises in MXene materials and also effectively prevents the recrystallization of potentially residual LiF during the film formation. Additionally, the utilization of this MXene electrode in an all-solid-state microsupercapacitor (MSC) with an interdigitated pattern demonstrates an exceptionally improved and stable electrochemical performance. This includes a high volumetric capacitance of approximately 467 F cm-3, an energy density of around 65 mWh cm-3, and impressive long-term cycle stability, retaining about 94% capacity after 10 000 cycles. Moreover, a downsized MSC device exhibits remarkable mechanical durability, retaining over 98% capacity even when folded and sustaining stability over extended periods. Therefore, we believe that this study provides valuable insights for advancing highly integrated energy storage devices, ensuring exceptional electrochemical efficiency and prolonged functionality in diverse environments, whether ambient or humid.

MXene/COFs membrane with sandwich structure for rapid salt/dye separation by layer-by-layer electrophoretic deposition

Covalent organic frameworks (COFs) have evolved into a transformative category of nanofiltration materials due to their intrinsic pore channels and high porosity, sparking a burgeoning interest in fully harnessing the potential of COFs for applications in nanofiltration. Herein, a sandwich structured MXene/COFs membrane was fabricated by the technique of layer-by-layer electrophoretic deposition (LBL EPD), with COFs nanospheres (COFs NPs) serving as the intermediate layer. During the EPD process, controlling the deposition time allows for convenient regulation of each layer's thickness, enabling rapid production of defect-free MXene/COFs membranes. The ultra-thin MXene layer offers excellent film-forming properties for COFs NPs, whereas the intermediate layer of COFs NPs plays a primary sieving function. Moreover, the pore-rich COFs NPs, the ultra-thin MXene layer, and the COFs NPs layer with abundant slits guarantee short and successive mass transport pathways. Under optimal conditions, the MXene/COFs membrane provided a permeance as high as 200.2 L‧m−2‧h−1‧bar−1 and a rejection rate of Congo red (CR) as high as 98.9 %. This exceptional performance holds steadfast even within pH ranges of 7–11 and during long-term operation. Meanwhile, MXene/COFs membranes exhibit commendable salt/dye separation performance, achieving an excellent separation factor of 121.1 for NaCl/CR. Moreover, the membrane's exceptional robustness and mechanical strength further facilitate its stable utilization under high transmembrane pressure (1–5 bar). To summarize, MXene/COFs membranes, characterized by their excellent nanofiltration and salt/dye separation performance, highlight the advantages of COFs within the nanofiltration field. This study introduces an innovative alternative approach to designing COFs membranes for highly efficient and high-precision molecular separations.

Noncontact Microfluidics of Highly Viscous Liquids for Accurate Self-Splitting and Pipetting.

Accurate dosing for various liquids, especially for highly viscous liquids, is fundamental in wide-ranging from molecular crosslinking to material processing. Despite droppers or pipettes being widely used as pipetting devices, they are powerless for quantificationally splitting and dosing highly viscous liquids (>100mPa s) like polymer liquids due to the intertwined macromolecular chains and strong cohesion energy. Here, a highly transparent photopyroelectric slippery (PS) platform is provided to achieve noncontact self-splitting for liquids with viscosity as high as 15000mPa s, just with the assistance of sunlight and a cooling source to provide a local temperature difference (ΔT). Moreover, to guarantee the accuracy for pipetting liquids (>80%), the ultrathin MXene film (within a thickness of 20nm) is self-assembled as the photo-thermal layers, overcoming the trade-off between transparency and photothermal property. Compared with traditional pipetting strategies (≈1.3% accuracy for pipetting polymer liquids), this accurate microfluidic chip shows great potential in adhesive systems (bonding strength, twice than using the droppers or pipettes).

Ultrasmall Pd nanocrystals confined into Co-based metal organic framework-decorated MXene nanoarchitectures for efficient methanol electrooxidation

The natural scarcity and insufficient utilization of noble metal-based catalysts bring a heavy block in the way of the widespread applications of direct methanol fuel cells. Herein, we propose a feasible bottom-up approach to the construction of ultrasmall Pd nanocrystals confined into Co-based metal organic framework-decorated Ti3C2Tx MXene (Pd/MOF-MX) nanoarchitectures via a controllable solvothermal process. The ultrathin MXene nanolamellas and porous Co-based MOFs constitute an ideal hybrid carrier with high electron conductivity and large accessible surface areas, which not only facilitates the size restriction and uniform dispersion of Pd nanocrystals, but also ameliorates their intrinsic catalytic activity through the direct electronic interactions. By virtue of the pronounced synergistic coupling effects, the newly-developed Pd/MOF-MX nanoarchitectures exhibit markedly enhanced electrocatalytic properties towards the methanol oxidation reaction, including a large electrochemically active surface area of 116.7 m2 g−1, a high mass activity of 1700.4 mA mg−1 as well as a satisfactory long-term durability, which are superior to those of traditional Pd electrocatalysts anchored on carbon blacks, carbon nanotubes, graphene, and undecorated MXene matrixes.

CO2-Philic Nanocomposite Polymer Matrix Incorporated with MXene Nanosheets for Ultraefficient CO2 Capture.

The incorporation of two-dimensional (2D) functional nanosheets in polymeric membranes is a promising material strategy to overcome their inherent performance trade-off behavior. Herein, we report a novel nanocomposite membrane design by incorporating MXene, a 2D sheet-like nanoarchitecture known for its advantageous lamellar morphology and surface functionalities, into a cross-linked polyether block amide (Pebax)/poly(ethylene glycol) methyl ether acrylate (PEGMEA) blend matrix, which delivered exceptional CO2/N2 and CO2/H2 separation performances that are critical to industrial CO2 capture applications. The finely dispersed Ti3C2Tx nanosheets in the blend polymer matrix led to an expansion of the free volume within the resultant mixed matrix membrane (MMM), giving rise to a substantially enhanced CO2 permeability of up to 1264.6 barrer, which is 102% higher than that of the pristine polymer. Moreover, these MXene-incorporated MMMs exhibited preferential sorption for CO2 over light gases, which contributed to an exceptional CO2/N2 and CO2/H2 selectivity (64.3 and 19.2, respectively) even at a small loading of only 1 wt %, allowing the overall performance to not only surpass the latest upper bounds but also exceed many previously reported high-performance nanosheet-based nanocomposite membranes. Long-term performance tests have also demonstrated the good stability of these membranes. This composite membrane design strategy reveals the remarkable potential of combining a blend copolymer matrix with ultrathin MXene nanosheets to achieve superior gas separation performance for environmentally important gas separations.

Ultrathin H-MXM as An "Ion Freeway" for High-Performance Osmotic Energy Conversion.

Nanofluidic membranes are currently being explored as potential candidates for osmotic energy harvesting. However, the development of high-performance nanofluidic membranes remains a challenge. In this study, the ultrathin MXene membrane (H-MXM) is prepared by ultrathin slicing and realize the ion horizontal transportation. The H-MXM membrane, with a thickness of only 3 µm and straight subnanometer channels, exhibits ultrafast ion transport capabilities resembling an "ion freeway". By mixing artificial seawater and river water, a power output of 93.6 Wm-2 is obtained. Just as cell membranes have an ultrathin thickness that allows for excellent penetration, this straight nanofluidic membrane also possesses an ultrathin structure. This unique feature helps to shorten the ion transport path, leading to an increased ion transport rate and improveS performance in osmotic energy conversion.

MXene-Based Mixed Conductor Interphase for Dendrite-Free Flexible Al Organic Battery.

Al batteries are promising post-Li battery technologies for large-scale energy storage applications owing to their low cost and high theoretical capacity. However, one of the challenges that hinder their development is the unsatisfactory plating/stripping of the Al metal anode. To circumvent this issue, an ultrathin MXene layer is constructed on the surface of Al by in situ chemical reactions at room temperature. The as-prepared flexible MXene film acts like armor to protect the Al-metal by its high ionic conductivity and high mechanical flexibility. The MXene endow the Al anode with a long cyclic life of more than 5000 h at ultrahigh current density of 50 mA cm-2 for Al//Al batteries and a retention of 100% over 200 cycles for 355 Wh kg-1 PTO//Al batteries. This work provides fresh insights into the formation and regulation of stable electrode-electrolyte interfaces as well as effective strategies for improving Al metal batteries.

Ultrathin MXene film interaction with electromagnetic radiation in the microwave range

The quick progress in communication technologies demands superior electromagnetic interference (EMI) shielding materials. However, achieving a high shielding effectiveness (SE) with thin films, which is needed for microscale, flexible, and wearable devices, through absorption of EM radiation remains a challenge. 2D titanium carbide MXene, Ti3C2Tx, has been shown to efficiently reflect electromagnetic waves. In this paper, we investigated the electromagnetic shielding of ultrathin printed Ti3C2Tx films and recorded absorption up to 50% for 4 nm-thick films. This behavior is explained by impedance matching. Analysis of the sheet impedance in the X-band frequency range allows us to correlate the EMI shielding mechanism with the electrical conductivity measured within the same range. The average bulk in-plane conductivity for 4 to 40 nm-thick films reaches 106 S/m, while the average relaxation time is estimated at around 2.3 ps. Our figures of merit are similar to those reported for ultrathin metal films, such as gold, showing that an abundant MXene material can replace noble metals. We demonstrate that the MXene conductivity mechanism does not change from direct current to THz. The conventional method of reporting EMI SE is correlated with absolute values of transmitted, reflected, and absorbed power, which allows us to interpret previous results on MXene EMI shielding. Considering the easy deposition of thin MXenes films from solution onto a variety of surfaces, our findings offer an attractive alternative for shielding microscale devices and personal electronics.

An Ultra-Thin MXene Film for Multimodal Sensing of Neuroelectrical Signals with Artifacts Removal.

Neuroelectrical signals transmitted onto the skin tend to decay to an extremely weak level, making them highly susceptible to interference from the environment and body movement. Meanwhile, for comprehensively understanding cognitive nerve conduction, multimodal sensing of neural signals, such as magnetic resonance imaging (MRI) and functional near-infrared spectroscopy (fNIRS), is highly required. Previous metal or polymer conductors cannot either provide a seamless on-skin feature for accurate sensing of neuroelectrical signals or be compatible with multimodal imaging techniques without opto- and magnet- artifacts. Herein, a ≈20nm thick MXene film that is able to simultaneously detect electrophysiological signals and perform imaging by MRI and fNIRS with high fidelity is reported. The ultrathin film is made of crosslinked Ti3 C2 Tx film via poly (3,4-ethylene dioxythiophene): polystyrene sulfonate (PEDOT:PSS), showing a record high electroconductivity and transparency combination (11000Scm-1 @89%). Among them, PEDOT: PSS not only plays a cross-linking role to stabilize MXene film but also shortens the interlayer distance for effective charge transfer and high transparency. Thus, it can achieve a low interfacial impedance with skin or neural surfaces for accurate recording of electrophysiological signals with low motion artifacts. Besides, the high transparency originating from the ultrathin feature leads to good compatibility with fNIRS and MRI without optical and magnetic artifacts, enabling multimodal cognitive neural monitoring during prolonged use.

Multifunctional Flexible MXene/AgNW Composite Thin Film with Ultrahigh Conductivity Enabled by a Sandwich-Structured Assembly Strategy.

Flexible composite films have attracted considerable attention due to great potential for healthcare, telecommunication, and aerospace. However, it is still challenging to achieve high conductivity and multifunctional integration, mainly due to poorly designed composite structures of these films. Herein, a novel sandwich-structured assembly strategy is proposed to fabricate flexible composite thin films made of Ag nanowire (AgNW) core and MXene layers by combination of spray coating and vacuum filtration process. In this case, ultrathin MXene layers play crucial roles in constructing compact composite structures strongly anchored to substrate with extensive hydrogen-bonding interactions. The resultant sandwich-structured MXene/AgNW composite thin films (SMAFs) exhibit ultrahigh electrical conductivity (up to 27193 S cm-1 ), resulting in exceptional electromagnetic interference shielding effectiveness of 16223.3 dB cm2 g-1 and impressive Joule heating performance with rapid heating rate of 10.4°C s-1 . Moreover, the uniform SMAFs can also be facilely cut into kirigami-patterned interconnects, which indicate superior strain-insensitive conductance even after long-term exposure to extreme temperatures. The demonstrated strategy offers a significant paradigm to construct multifunctional composite thin films for next-generation integrated flexible electronics with practical applications.

Reinforcing and toughening bacterial cellulose/MXene films assisted by interfacial multiple cross-linking for electromagnetic interference shielding and photothermal response

Ultrathin MXene composite films, with their flexibility, metal-level conductivity, and multifunction compatibility, are an ideal choice for electromagnetic interference (EMI) shielding materials in future developments. Nonetheless, the dilemma between electrical conductivity and robustness in these composite films remains a challenge. Herein, an ammonium polyphosphate (APP) assisted interfacial multiple cross-linking strategy, achieved via simple solution blending and filtration, was employed to reinforce and toughen the “brick–mortar” layered MXene/bacterial cellulose (MBCA) films without compromising their conductivity and EMI shielding ability. The introduction of a small amount of APP leads to multiple interfacial interactions between MXene and bacterial cellulose, resulting in significant enhancements in mechanical strength (360.8 MPa), Young's modulus (2.8 GPa), fracture strain (17.3%), and toughness (34.1 MJ/m3). Concurrently, the MBCA film displayed satisfactory conductivity values of 306.7 S/cm and an EMI SE value of 41 dB upon optimizing the MXene content. Additionally, the MBCA film demonstrated a consistent, rapid-response photothermal conversion capability, achieving a photothermal conversion temperature of 97 °C under a light intensity of 200 mW/m2. Consequently, this tough and multifunctional EMI shielding film holds substantial promise for protecting electronic equipment.

Ultrathin Ti3C2Tx MXene sheets with high electrochemically active area anchored Pt boosting hydrogen evolution

To reduce platinum usage, ultrathin MXene sheets with little restacking effect were prepared. The ultrathin MXene was prepared by a two-step etching process, which showed high specific surface area with low charge transfer resistance. The sample showed a double layer capacity of 64.98 mF cm−2, which is 14 times as large as that of ordinary HF prepared MXene, indicating a larger electrochemically active surface area. It showed a much better HER performance of ∼190 mV at 10 mA cm−2. The better performance attributes to 0.4 wt% Pt loaded. The Pt loaded MXene exhibited a better HER performance of ∼75 mV at 10 mA cm−2 and a Tafel slope of 61.7 mV·dec−1 close to 40 wt% commercial Pt/C. The sample performed better than Pt/C in a 3 h chronopotentiometry test and hardly changed in ECSA after the cyclic experiment. With more Pt loading, the sample delivered better HER performance than Pt/C in the LSV test (∼51 mV at 10 mA cm−2). This work provides an effective route for the preparation of ultrathin MXene sheets with larger electrochemically active area and more active sites for Pt loading, leading to superior HER performance.

Transversal nanochannel-enabled MXene laminated membranes for superior oil-water separation: A fluid mosaic cytomembrane inspired approach

Transition metal carbide and nitride materials (MXenes) have been greatly appreciated for their facilely exfoliated and hydrophilic two-dimensional (2D) layered structure to fabricate laminated membranes for oil separation. However, the denser slits and longer interlayer transport of traditional MXene membranes usually result in the poor permeability and antifouling performance. Herein, a novel approach was developed by synthesizing ultra-thin MXene and ferroferric oxide doped molybdenum disulfide (FM) and subsequently embedding FM into MXene laminates. This method yielded additional transversal nanochannels that enable lateral transport in a manner akin to that of a mosaic transport protein. Additionally, the incorporation of FM resulted in the creation of extremely irregular surfaces that form extensive membrane structures, reminiscent of tightly packed phospholipid bilayers. The incorporation of flower-like FM composites with MXene laminates endowed the resultant membrane with improved interface hydrophilicity, intensive surface roughness and enhanced permeability. These effects synergistically contributed to an exceptionally high pure water flux of the resultant membrane (3.12 × 104 L m−2 h−1), surpassing that of the control membrane (6.15 × 103 L m−2 h−1) without FM by over 5-fold. Furthermore, the optimum membrane exhibited enhanced permeance to oil mixtures (3.75 × 103 L m−2 h−1) and emulsions (4.25 × 102 L m−2 h−1), with separation of over 99% remaining. Impressively, the permeability of severely fouled membranes could be restored by 99% under visible light, highlighting the admirable photocatalytic self-cleaning ability enabled by MXene and FM. The underlying mechanisms that account for the superior antifouling performance and self-cleaning ability of the laminated membrane were also elucidated by the extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory. The facile fabrication strategy employing transversal transport laminates provides a remarkable approach for water purification and other fluidic separation applications.

The performances and mechanisms for Cr(VI) and Cr(III) removal using TMAOH delaminated Ti3C2Tx suspension

Ultra-thin MXene nanosheets (Nss) were facilely prepared via delaminating and intercalating the multi-layered MXene using tetramethylammonium hydroxide (TMAOH). Electron-rich characteristics, abundant surface active sites and the negative charges made MXene Nss having both good reduction ability and adsorption capacities, which would effectively remove anion Cr(VI) via reduction and remove cation Cr(III) via adsorption. Batch adsorption tests were carried out to study the pH impact, adsorption kinetics and isotherms. Upon adsorption, the well dispersed MXene Nss suspension was aggregated to form flocs and sediment at the bottom. The maximum Cr(VI) and Cr(III) removing capacities are calculated to be 554.9 mg/g at 318 K and 283 mg/g at 298 K, respectively. The mechanisms on Cr(VI)/Cr(III) adsorption were well studied employing SEM, TEM, XPS and FT-IR. In addition, the MXene Nss also showed good adsorption capacity towards other metal cations (such as Cu2+, Cd2+, and Pb2+), manifesting that the current MXene Nss has the potential to be used as a general-purpose adsorbent.

Ultrathin MXene nanosheet-based TiO2/CdS heterostructure as a photoelectrochemical sensor for detection of CEA in human serum samples

To develop highly accurate and ultrasensitive strategies is of great importance for the clinical measurement, in particular, the detection of cancer biomarkers. Herein, we synthesized an ultrasensitive TiO2/MXene/CdS QDs (TiO2/MX/CdS) heterostructure as a photoelectrochemical immunosensor, which favors energy levels matching and fast electron transfer from CdS to TiO2 in the help of ultrathin MXene nanosheet. Dramatic photocurrent quenching can be observed upon incubation of the TiO2/MX/CdS electrode by Cu2+ solution from 96-well microplate, which caused by the formation of CuS and subsequent CuxS (x = 1, 2), reducing the absorption of light and boosting the electron-hole recombination upon irradiation. As a result, the as-prepared biosensor demonstrates a linearly increased photocurrent quenching percentage (Q%) value with CEA concentration ranging from 1 fg/mL to 10 ng/mL, as well as a low detection limit of 0.24 fg/mL. Benefit from its excellent stability, high selectivity and good reproducibility of as-prepared PEC immunosensor, we believe that this proposed strategy might provide new opportunities for clinical diagnosis of CEA and other tumor markers.

Giant piezoionic effect of ultrathin MXene nanosheets toward highly-sensitive sleep apnea diagnosis

Flexible piezoionic sensors are emerging as an important platform for non-invasive human health detections. But it keeps a long way toward applications because of the weak piezoionic effects of general sensing materials. Here, we report giant piezoionic effect of ultrathin MXene nanosheets, which is enabled by abundant ion channels and strong ionic affinity. The flexible sensor delivers a high piezoionic signal of 219 mV, which significantly exceeds those of the best-known piezoionic materials. It displays superior working stability with signal retention of 98% even after 10,000 cycles under ambient conditions. The piezoionic sensors display high sensitivity for recognising physiological signals of human body, including wrist bendings, exercise modes, and pulse vibrations. Especially, sleep apnea diagnosis, which is vital for sleep-related disease, can be real-time detected accurately and reliably based on the flexible sensors. The discovery of giant piezoionic effects for sensitive health detections will accelerate development of smart medical instruments.

Constructing reduced porous graphene oxide for tailoring mass-transfer channels in ultrathin MXene (Ti3C2Tx) membranes for efficient dye/salt separation

Two-dimensional (2D) membranes such as graphene oxide (GO) and MXene have attracted increasing interest in water purification. Critical challenges that impede their performance in separation applications include poor stability (swelling), low mass-transfer rate (high tortuosity), and an unavoidable trade-off between permeability and selectivity. Herein, we propose an effective multidimensional channel design strategy for preparing high-performance 2D composite membranes, featuring robust and abundant mass transfer channels. Specifically, reduced porous GO (rPGO) with high-density nanopores (size: ca. 14.7 nm, density: ca. 2.2 × 1014 m−2) and a few oxygen-containing functional groups were rationally designed and then deployed as multifunctional intercalators in MXene interlayers (rPGO-MXene, rPGM) to construct highly permeable, in-plane nanochannels and stable and tunable interlayer sieve channels. The intercalation of tailorable rPGO provides additional transport channels and weakens the interlayer repulsive hydration force, yielding composite membranes with remarkably enhanced water permeability and anti-swelling properties. As a result, the optimized membrane (10 % rPGM) exhibited an outstanding water permeability of 198.8 L m−2h−1 bar−1, 100 % rejection of Congo red, 5.3 % rejection of NaCl, and satisfactory stability (30 h) under cross-flow separation conditions. This study provides an innovative and facile approach for designing robust 2D membranes with abundant permeable nanochannels for highly efficient and precise molecular separation.