3D Macroscopic Architectures from Self‐Assembled MXene Hydrogels

Assembly of 2D MXene sheets into a 3D macroscopic architecture is highly desirable to overcome the severe restacking problem of 2D MXene sheets and develop MXene‐based functional materials. However, unlike graphene, 3D MXene macroassembly directly from the individual 2D sheets is hard to achieve for the intrinsic property of MXene. Here a new gelation method is reported to prepare a 3D structured hydrogel from 2D MXene sheets that is assisted by graphene oxide and a suitable reductant. As a supercapacitor electrode, the hydrogel delivers a superb capacitance up to 370 F g^?1 at 5 A g^?1, and more promisingly, demonstrates an exceptionally high rate performance with the capacitance of 165 F g^?1 even at 1000 A g^?1. Moreover, using controllable drying processes, MXene hydrogels are transformed into different monoliths with structures ranging from a loosely organized porous aerogel to a dense solid. As a result, a 3D porous MXene aerogel shows excellent adsorption capacity to simultaneously remove various classes of organic liquids and heavy metal ions while the dense solid has excellent mechanical performance with a high Young's modulus and hardness.     

Conductive MXene Nanocomposite Organohydrogel for Flexible,Healable, Low‐Temperature Tolerant Strain Sensors

Conductive hydrogels are attracting tremendous interest in the field of flexible and wearable soft strain sensors because of their great potential in electronic skins, and personalized healthcare monitoring. However, conventional conductive hydrogels using pure water as the dispersion medium will inevitably freeze at subzero temperatures, resulting in the diminishment of their conductivity and mechanical properties; meanwhile, even at room temperature, such hydrogels suffer from the inevitable loss of water due to evaporation, which leads to a poor shelf‐life. Herein, an antifreezing, self‐healing, and conductive MXene nanocomposite organohydrogel (MNOH) is developed by immersing MXene nanocomposite hydrogel (MNH) in ethylene glycol (EG) solution to replace a portion of the water molecules. The MNH is prepared from the incorporation of the conductive MXene nanosheet networks into hydrogel polymer networks. The as‐prepared MNOH exhibits an outstanding antifreezing property (?40 °C), long‐lasting moisture retention (8 d), excellent self‐healing capability, and superior mechanical properties. Furthermore, this MNOH can be assembled as a wearable strain sensor to detect human biologic activities with a relatively broad strain range (up to 350% strain) and a high gauge factor of 44.85 under extremely low temperatures. This work paves the way for potential applications in electronic skins, human?machine interactions, and personalized healthcare monitoring.     

Precious‐Metal‐Free Electrocatalysts for Activation of Hydrogen Evolution with Nonmetallic Electron Donor: Chemical Composition Controllable Phosphorous Doped Vanadium Carbide MXene

The insufficient strategies to improve electronic transport, the poor intrinsic chemical activities, and limited active site densities are all factors inhibiting MXenes from their electrocatalytic applications in terms of hydrogen production. Herein, these limitations are overcome by tunable interfacial chemical doping with a nonmetallic electron donor, i.e., phosphorization through simple heat‐treatment with triphenyl phosphine (TPP) as a phosphorous source in 2D vanadium carbide MXene. Through this process, substitution, and/or doping of phosphorous occurs at the basal plane with controllable chemical compositions (3.83–4.84 at%). Density functional theory (DFT) calculations demonstrate that the P? C bonding shows the lowest surface formation energy (ΔG_Surf) of 0.027 eV Å^?2 and Gibbs free energy (ΔG_H) of –0.02 eV, whereas others such as P‐oxide and P? V (phosphide) show highly positive ΔG_H. The P3–V₂CT_x treated at 500 °C shows the highest concentration of P? C bonds, and exhibits the lowest onset overpotential of –28 mV, Tafel slope of 74 mV dec^?1, and the smallest overpotential of ‐163 mV at 10 mA cm^?2 in 0.5 m H₂SO₄. The first strategy for electrocatalytically accelerating hydrogen evolution activity of V₂CT_x MXene by simple interfacial doping will open the possibility of manipulating the catalytic performance of various MXenes.     

Reversible Crumpling of 2D Titanium Carbide (MXene) Nanocoatings for Stretchable Electromagnetic Shielding and Wearable Wireless Communication

In the emerging Internet of Things, stretchable antennas can facilitate wireless communication between wearable and mobile electronic devices around the body. The proliferation of wireless devices transmitting near the human body also raises interference and safety concerns that demand stretchable materials capable of shielding electromagnetic interference (EMI). Here, an ultrastretchable conductor is fabricated by depositing a crumple‐textured coating composed of 2D Ti₃C₂T_x nanosheets (MXene) and single‐walled carbon nanotubes (SWNTs) onto latex, which can be fashioned into high‐performance wearable antennas and EMI shields. The resulting MXene‐SWNT (S‐MXene)/latex devices are able to sustain up to an 800% areal strain and exhibit strain‐insensitive resistance profiles during a 500‐cycle fatigue test. A single layer of stretchable S‐MXene conductors demonstrate a strain‐invariant EMI shielding performance of ≈30 dB up to 800% areal strain, and the shielding performance is further improved to ≈47 and ≈52 dB by stacking 5 and 10 layers of S‐MXene conductors, respectively. Additionally, a stretchable S‐MXene dipole antenna is fabricated, which can be uniaxially stretched to 150% with unaffected reflected power <0.1%. By integrating S‐MXene EMI shields with stretchable S‐MXene antennas, a wearable wireless system is finally demonstrated that provides mechanically stable wireless transmission while attenuating EM absorption by the human body.     

2D/2D 1T‐MoS2/Ti3C2 MXene Heterostructure with Excellent Supercapacitor Performance

2D/2D heterostructures can combine the collective advantages of each 2D material and even show improved properties from synergistic effects. 2D Transition metal carbide Ti₃C₂ MXene and 2D 1T‐MoS₂ have emerged as attractive prototypes in electrochemistry due to their rich properties. Construction of these two 2D materials, as well as investigation about synergistic effects, is absent due to the instability of 1T‐MoS₂. Here, 3D interconnected networks of 1T‐MoS₂/Ti₃C₂ MXene heterostructure are constructed by magneto‐hydrothermal synthesis, and the electrochemical storage mechanisms are investigated. Improved extra capacitance is observed due to enlarged ion storage space from a synergistically interplayed effect in 3D interconnected networks. Outstanding rate performance is realized because of ultrafast electron transport originating from Ti₃C₂ MXene. This work provides an archetype to realize excellent electrochemical properties in 2D/2D heterostructures.     

MXene Composite and Coaxial Fibers with High Stretchability and Conductivity for Wearable Strain Sensing Textiles

The integration of nanomaterials with high conductivity into stretchable polymer fibers can achieve novel functionalities such as sensing physical deformations. With a metallic conductivity that exceeds other solution‐processed nanomaterials, 2D titanium carbide MXene is an attractive material to produce conducting and stretchable fibers. Here, a scalable wet‐spinning technique is used to produce Ti₃C₂T_x MXene/polyurethane (PU) composite fibers that show both conductivity and high stretchability. The conductivity at a very low percolation threshold of ≈1 wt% is demonstrated, which is lower than the previously reported values for MXene‐based polymer composites. When used as a strain sensor, the MXene/PU composite fibers show a high gauge factor of ≈12900 (≈238 at 50% strain) and a large sensing strain of ≈152%. The cyclic strain sensing performance is further improved by producing fibers with MXene/PU sheath and pure PU core using a coaxial wet‐spinning process. Using a commercial‐scale knitting machine, MXene/PU fibers are knitted into a one‐piece elbow sleeve, which can track various movements of the wearer's elbow. This study establishes fundamental insights into the behavior of MXene in elastomeric composites and presents strategies to achieve MXene‐based fibers and textiles with strain sensing properties suitable for applications in health, sports, and entertainment.     

Janus‐Structured Co‐Ti3C2 MXene Quantum Dots as a Schottky Catalyst for High‐Performance Photoelectrochemical Water Oxidation

MXene materials have attracted increasing attention in electrochemical energy‐storage applications while MXene also becomes photo‐active at the quantum dot scale, making it an alternative for solar‐energy‐conversion devices. A Janus‐structured cobalt‐nanoparticle‐coupled Ti₃C₂ MXene quantum dot (Co‐MQD) Schottky catalyst with tunable cobalt‐loading content serving as a photoelectrochemical water oxidation photoanode is demonstrated. The introduction of cobalt triggers concomitant surface‐plasmon effects and acts as a water oxidation center, enabling visible‐light harvesting capability and improving surface reaction kinetics. Most importantly, due to the rectifying effects of Co‐MQD Schottky junctions, photogenerated carrier separation/injection efficiency can be fundamentally facilitated. Specifically, Co‐MQD‐48 exhibits both superior photoelectrocatalysis (2.99 mA cm^?2 at 1.23 V vs RHE) and charge migration performance (87.56%), which corresponds to 194% and 236% improvement compared with MQD. Furthermore, excellent photostability can be achieved with less than 6.6% loss for 10 h cycling reaction. This fills in gaps in MXene material research in photoelectrocatalysis and allows for the extension of MXene into optical‐related fields.     

SnO-SnO2 modified two-dimensional MXene Ti3C2Tx for acetone gas sensor working at room temperature

Acetone,as widely used reagents in industry and laboratories,are extremely harmful to the human.So the detection of acetone gas concentrations and leaks in special environments at room temperature is essential.Herein,the nanocomposite combining SnO-SnO2 (p-n junction) and Ti3C2Tx MXene was successfully synthesized by a one-step hydrothermal method.Because of the existence of a small amount of oxygen during the hydrothermal conditions,part of the p-type SnO was oxidized to n-type SnO2,forming in-situ p-n junctions on the surface of SnO.The hamburger-like SnO-SnO2/Ti3C2Tx sensor exhibited improved acetone gas sensing response of 12.1 (Rg/Ra) at room temperature,which were nearly 11 and 4 times higher than those of pristine Ti3C2Tx and pristine SnO-SnO2,respectively.Moreover,it expressed a short recovery time (9 s) and outstanding reproducibility.Because of the different work functions,the Schottky barrier was formed between the SnO and the Ti3C2Tx nanosheets,acting as a hole accumulation layer (HALs) between Ti3C2Tx and tin oxides.Herein,the sensing mechanism based on the formation of hetero-junctions and high conductivity of the metallic phase of Ti3C2Tx MXene in SnO-SnO2/Ti3C2Tx sensors was discussed in detail.     

Enhanced Q-switching performance of magnetite nanoparticle via compositional engineering with Ti3C2 MXene in the near infrared region

In this work,we reported a new strategy to improve the nonlinear saturable absorption performance of magnetite (Fe3O4) nanoparticles (FONPs) via the compositional engineering with the Ti3C2 MXene in the near-infrared (NIR) region.Based on the DFT simulation,the band structures and work function were significantly modified by the Ti3C2 MXene doping.By using the open-aperture Z-scan technology,the nonlinear optical features of the FONPs@Ti3C2 nanocomposite were significantly improved,show-ing the great potential as the saturable absorber in the pulsed laser.With the nanocomposite as the saturable absorber,the passively Q-switched Nd∶GdVO4 lasers emitted much shorter pulse durations when compared with the pristine FONP saturable absorber.These findings indicated that FONPs@Ti3C2 heterostructure was a promising saturable absorber for the short pulse generation in the NIR region.