Preparation of branched polyethyleneimine-assisted boronic acid-functionalized magnetic MXene for the enrichment of catecholamines in urine samples.

Herein, a magnetic borate-functionalized MXene composite with multiple boronic affinity sites was fabricated by embedding Fe3 O4 nanoparticles with 4-formylphenylboronic acid functionalized Ti3 C2 Tx nanosheets and served as sorbent for the simultaneous extraction of catecholamines (CAs) in urine samples. The morphology and structure of the magnetic materials were investigated using scanning microscopy, vibrating sample magnetometer, X-ray photoelectron spectrometer, and X-ray diffraction. The introduction of polyethyleneimine can amplify the bonded boronic acid groups, thereby effectively improving the adsorption capacities for CAs based on the multiple interactions of boronic affinity, hydrogen bonding, and metal coordination. The adsorption performance was investigated using the kinetics and isotherms models, and the main parameters that influence the extraction efficiency were optimized. Under the most favorable magnetic solid-phase extraction condition, a sensitive method for the analysis of CAs in urine samples was developed by combining magnetic solid-phase extraction conditions with high-performance liquid chromatography detection. The findings illustrated that the proposed approach possessed a wide linearity range of 0.05-250 ng/mL with an acceptable correlation coefficient (R2  ≥ 0.9984) and detection limits of 0.010-0.015 ng/mL for the target CAs. The research not only provides a notable composite with multiple boronic affinity sites but also offers an effective and feasible measure for the detection of CAs in biological samples.

Boron Quantum Dots Pillared Ti3 C2 Tx Membrane Electrode with High Rate Performance for Supercapacitor.

A sonication-assisted liquid-phase preparation technique is developed to prepare boron quantum dots (BQDs) with a lateral size of 3 nm in a solution of NMP and NBA; it shows a direct bandgap semiconductor with a bandgap of 3 eV and a specific capacitance of 41 F g-1 . A BQDs(10)-Ti3 C2 Tx membrane electrode with excellent capacitance and high flexibility is prepared by using Ti3 C2 Tx nanosheets (NSs) as assembled units and BQDs as pillar; it gives a specific capacitance of 524 F g-1 at 1 A g-1 in 6 m H2 SO4 electrolyte, a high capacity retention of 75%, and a minimum relaxation time of 0.51 s. An all-solid-state BQDs(10)-Ti3 C2 Tx flexibility supercapacitor is assembled by using a BQDs(10)-Ti3 C2 Tx membrane as electrodes and PVA/H2 SO4 hydrogel as electrolyte; it not only shows an area specific capacitance of 552 mF cm-2 at 1.25 mA cm-2 , a retention rate of 75%, a capacity retention of 93% after 5000 cycles, and an energy density of 40.4 Wh cm-3 at a volume power density of 416 W cm-3 , but also provides superior flexibility and can be bent to different degrees, showing that the assembled BQDs(10)-Ti3 C2 Tx membrane electrode and BQDs(10)-Ti3 C2 Tx flexible supercapacitor display broad application prospects in field of portable/wearable electronic devices.

Construction of a Two-Dimensional GO/Ti3C2TX Composite Membrane and Investigation of Mg2+/Li+ Separation Performance.

Graphene oxide (GO) two-dimensional (2D) membranes with unique layer structures and tunable layer spacing have special advantages and great potential in the field of water treatment. However, GO membranes face the issues of weak anti-swelling ability as well as poor permeability. We prepared GO/Ti3C2TX 2D composite membranes with 2D/2D structures by intercalating Ti3C2TX nanosheets with slightly smaller sizes into GO membranes. Ti3C2TX intercalation can effectively expand the layer spacing of GO, thereby substantially enhancing the flux of the composite membrane (2.82 to 6.35 L·m-2·h-1). Moreover, the GO/Ti3C2TX composite membrane exhibited a good Mg2+/Li+ separation capability. For the simulated brine, the separation factor of M2 was 3.81, and the salt solution flux was as high as 5.26 L·m-2·h-1. Meanwhile, the incorporation of Ti3C2TX nanosheets significantly improved the stability of GO/Ti3C2TX membranes in different pH environments. This study provides a unique insight into the preparation of highly permeable and ion-selective GO membranes.

Schottky Junction Nanozyme Based on Mn-Bridged Co-Phthalocyanines and Ti3C2Tx Nanosheets Boosts Integrative Type I and II Photosensitization for Multimodal Cancer Therapy.

Cancer phototheranostics have the potential for significantly improving the therapeutic effectiveness, as it can accurately diagnose and treat cancer. However, the current phototheranostic platforms leave much to be desired and are often limited by tumor hypoxia. Herein, a Schottky junction nanozyme has been established between a manganese-bridged cobalt-phthalocyanines complex and Ti3C2Tx MXene nanosheets (CoPc-Mn/Ti3C2Tx), which can serve as an integrative type I and II photosensitizer for enhancing cancer therapeutic efficacy via a photoacoustic imaging-guided multimodal chemodynamic/photothermal/photodynamic therapy strategy under near-infrared (808 nm) light irradiation. The Schottky junction not only possessed a narrow-bandgap, enhanced electron-hole separation ability and exhibited a potent redox potential but also enabled improved H2O2 and O2 supplying performances in vitro. Accordingly, the AS1411 aptamer-immobilized CoPc-Mn/Ti3C2Tx nanozyme illustrated high accuracy and excellent anticancer efficiency through a multimodal therapy strategy in in vitro and in vivo experiments. This work presents a valuable method for designing and constructing a multifunctional nanocatalytic medicine platform for synergistic cancer therapy of solid tumors.

Biotransformation of 2D Nanomaterials through Stimulated Bacterial Respiration-Produced Extracellular Reactive Oxygen Species: A Common but Overlooked Process.

The biotransformation of 2D nanomaterials is still poorly understood, although their environmental fates are becoming an increasing concern with their broad applications. Here, we found that Ti3C2Tx nanosheets, a typical 2D nanomaterial, could be oxidized by reactive oxygen species (ROS) produced by both Gram-negative (Escherichia coli and Shewanella oneidensis) and Gram-positive (Bacillus subtilis) bacteria, with the formation of titanium dioxide (TiO2) on the nanosheet surfaces and impairment of structural integrity. Specifically, Ti3C2Tx nanosheets stimulated bacterial respiration Complex I, leading to increased generation of extracellular O2•- and the formation of H2O2 and •OH via Fenton-like reactions, which intensified the oxidation of the nanosheets. Surface modifications with KOH and hydrazine (HMH), especially HMH, could limit bacterial oxidation of the nanosheets. These findings reveal a common but overlooked process in which oxygen-respiring bacteria are capable of oxidizing 2D nanosheets, providing new knowledge for environmental fate evaluation and future design of functional 2D nanomaterials.

Efficient Two-Dimensional Perovskite Solar Cells Realized by Incorporation of Ti3C2Tx MXene as Nano-Dopants.

Two-dimensional (2D) perovskites solar cells (PSCs) have attracted considerable attention owing to their excellent stability against humidity; however, some imperfectness of 2D perovskites, such as poor crystallinity, disordered orientation, and inferior charge transport still limit the power conversion efficiency (PCE) of 2D PSCs. In this work, 2D Ti3C2Tx MXene nanosheets with high electrical conductivity and mobility were employed as a nanosized additive to prepare 2D Ruddlesden-Popper perovskite films. The PCE of solar cells was increased from 13.69 (without additive) to 15.71% after incorporating the Ti3C2Tx nanosheets with an optimized concentration. This improved performance is attributed to the enhanced crystallinity, orientation, and passivated trap states in the 3D phase that result in accelerated charge transfer process in vertical direction. More importantly, the unencapsulated cells exhibited excellent stability under ambient conditions with 55 ± 5% relative humidity.

Superior Wear-Resistance of Ti3C2Tx Multilayer Coatings.

Owing to MXenes' tunable mechanical properties induced by their structural and chemical diversity, MXenes are believed to compete with state-of-the-art 2D nanomaterials such as graphene regarding their tribological performance. Their nanolaminate structure offers weak interlayer interactions and an easy-to-shear ability to render them excellent candidates for solid lubrication. However, the acting friction and wear mechanisms are yet to be explored. To elucidate these mechanisms, 100-nm-thick homogeneous multilayer Ti3C2Tx coatings are deposited on technologically relevant stainless steel by electrospraying. Using ball-on-disk tribometry (Si3N4 counterbody) with acting contact pressures of about 300 MPa, their long-term friction and wear performance under dry conditions are studied. MXene-coated specimens demonstrate a 6-fold friction reduction and an ultralow wear rate (4 × 10-9 mm3 N-1 m-1) over 100 000 sliding cycles, outperforming state-of-the-art 2D nanomaterials by at least 200% regarding their wear life. High-resolution characterization verified the formation of a beneficial tribolayer consisting of thermally/mechanically degraded MXenes and amorphous/nanocrystalline iron oxides. The transfer of this tribolayer to the counterbody transforms the initial steel/Si3N4 contact to tribolayer/tribolayer contact with low shear resistance. MXene pileups at the wear track's reversal points continuously supply the tribological contact with fresh, lubricious nanosheets, thus enabling an ultra-wear-resistant and low-friction performance.

Enhanced Electromagnetic Wave-Absorbing Performance of Magnetic Nanoparticles-Anchored 2D Ti3C2Tx MXene.

Two-dimensional Ti3C2Tx MXene-based hybrids-anchored magnetic metal nanoparticles show a huge potential application as effective wave absorbers due to the synergistic electromagnetic (EM) loss effect. In this work, uniform and size-controllable nickel, cobalt, or nickel-cobalt alloy nanoparticles were in situ grown on the surface of MXene via a facile and moderate co-solvothermal method for the first time. As an example, a nickel nanoparticles-anchored MXene (Ni@MXene) hybrid was homodispersed into dielectric polyvinylidene fluoride to develop its EM wave-absorbing capacity to a great extent. As expected, the results showed strong reflection loss (RLmin = -52.6 dB at 8.4 GHz), broad effective absorption bandwidth (EAB = 3.7 GHz including 71% of X-band), low loading (10 wt % Ni@MXene), and thin thickness (3.0 mm). By adjusting the sample thickness, EAB can cover completely the whole X-band with a maximum of 6.1 GHz, showing a huge potential of Ni@MXene hybrid applying as aircraft stealth coating. The mechanism analyses revealed that the excellent impedance matching, magnetocoupling effect, conductance, magnetic loss, and multiple scatterings contribute to the splendid EM wave-absorbing performance of the Ni@MXene hybrid. Considering the excellent overall performance, the Ni@MXene hybrid was identified as a promising candidate for EM wave absorption.

Solution-Plasma-Assisted Bimetallic Oxide Alloy Nanoparticles of Pt and Pd Embedded within Two-Dimensional Ti3C2T x Nanosheets as Highly Active Electrocatalysts for Overall Water Splitting.

Exploiting high-efficiency and low-cost bifunctional electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) has been actively encouraged because of their potential applications in the field of clean energy. In this paper, we reported a novel electrocatalyst based on an exfoliated two-dimensional (2D) MXene (Ti3C2T x) loaded with bimetallic oxide alloy nanoparticles (NPs) of Pt and Pd (represented by PtO aPdO bNPs@Ti3C2T x), which was synthesized via solution plasma (SP) modification. The prepared materials were then utilized as highly efficient bifunctional electrocatalysts toward the HER and OER in alkaline solution. At a high plasma input power (200 W), bimetallic oxide alloy nanoparticles of Pt and Pd or nanoclusters with different metallic valence states were deposited onto the Ti3C2T x nanosheets. Because of the synergism of the noble-metal NPs and the Ti3C2T x nanosheets, the electrocatalytic results revealed that the as-prepared PtO aPdO bNPs@Ti3C2T x nanosheets under the plasma input power of 200 W for 3 min only required a low overpotential to attain 10 mA cm-2 for the HER (-26.5 mV) in 0.5 M H2SO4 solution and OER (1.54 V) in 0.1 M KOH solution. Moreover, water electrolysis using this catalyst achieved a water splitting current density of 10 mA cm-2 at a low cell voltage of 1.53 V in 1.0 M KOH solution. These results suggested that the hybridization of the extremely low usage of PtO a/PdO b NPs (1.07 µg cm-2) and Ti3C2T x nanosheets by SP will expand the applications of other clean energy reactions to achieve sustainable energy.