Ti3 C2 Tx Research Articles

Oxygen-Vacancy-Induced Formation of Pt-Based Intermetallics on MXene with Strong Metal-Support Interactions for Efficient Oxygen Reduction Reaction.

The Pt-based alloys can moderate the binding energies of oxygenated species on the catalytic surface, endowing the superior catalytic performance towards oxygen reduction reaction (ORR). Nevertheless, it is still challenging to explore general methods to synthesize structurally ordered intermetallics with uniform distributions. Herein, the strong metal-support interaction is employed to facilitate the interdiffusion of Pt/M atoms by establishing a tunnel of oxygen vacancy on ultrathin Ti3C2Tx (MXene) sheets, synthesizing the ordered PtFe, PtCo, PtZn, PdFe, PdZn intermetallics loaded onto Ti3C2Tx. Furthermore, the in-situ generation of Ti-O from Ti3C2Tx could be bonded with Pt and forming Pt-O-Ti, resulting in charge redistribution through Pt-O-Ti structure. Theoretical calculations demonstrate that the valuable charge redistribution can be observed at the interface and extended even to at the distance of two nanometers from the interface, which can modulate the Pt-Pt distance, optimize Pt-O binding energy and enhance intrinsic activity towards ORR. The strong coupling interaction between PtFe and Ti3C2Tx containing the titanium oxide layer endows the high stability of the composites. This work not only presents a general synthesis strategy for intermetallics but also provides a new insight that metal-support interaction is essential for the structural evolution of intermetallics on materials with oxygen vacancies.

A Near-Infrared Photothermal-Responsive Underwater Adhesive with Tough Adhesion and Antibacterial Properties.

Developing tunable underwater adhesives that possess tough adhesion in service and easy detachment when required remains challenging. Herein, a strategy is proposed to design a near infrared (NIR) photothermal-responsive underwater adhesive by incorporating MXene (Ti3C2Tx)-based nanoparticles within isocyanate-modified polydimethylsiloxane (PDMS) polymer chains. The developed adhesive exhibits long-term and tough adhesion with an underwater adhesion strength reaching 5.478MPa. Such strong adhesion is mainly attributed to the covalent bonds and hydrogen bonds at the adhesive-substrate interface. By making use of the photothermal-response of MXene-based nanoparticles and the thermal response of PDMS-based chains, the adhesive possesses photothermal-responsive performance, exhibiting sharply diminished adhesion under NIR irradiation. Such NIR-triggered tunable adhesion allows for easy and active detachment of the adhesive when needed. Moreover, the underwater adhesive exhibits photothermal antibacterial property, making it highly desirable for underwater applications. This work enhances the understanding of photothermal-responsive underwater adhesion, enabling the design of tunable underwater adhesives for biomedical and engineering applications.

Pillar-Structured Ti3 C2 Tx MXene with Engineered Interlayer Spacing for High-Performance Magnesium Batteries.

Two-dimentional (2D)Ti3 C2 Tx MXene has attracted significant attention in non-lithium-ion batteries due to its excellent electrical conductivity, high volumetric capacity, and ability to accommodate intercalants. Rechargeable magnesium batteries with Mg metal anodes are noted for their high theoretical energy density, potential safety, earth abundance, dendrite-free Mg2+ plating/stripping mechanism on the anode side, and low cost. Nevertheless, owing to the large polarity of divalent Mg2+ ions, the insertion of Mg2+ into the MXene layers suffers from sluggish kinetics, limiting the performance for storage of Mg2+ ions. Herein, a simple self-assembly strategy is demonstrated to achieve high magnesium ion storage capability with pillar-structured Ti3 C2 Tx MXene by intercalating a hyperbranched polyethylene ionomer containing quaternary ammonium ions. The ionomer intercalation/modification leads to the expansion of interlayer spacing of the MXene and, meanwhile, improves its affinity to low-polarity THF-based electrolyte.The delaminated ionomer-modified MXene shows significantly improved electrochemical performance as a cathode material for Mg batteries. It shows a promising cycling stability with a capacity retention of 86% after 400 cycles at 200mAg-1 , as well as outstanding high-rate performance with a capacity of 110mAhg-1 retained at 1,000mAg-1 relative to 213mAhg-1 at 20mAg-1 .

Construction of Nickel Molybdenum Sulfide/Black Phosphorous 3D Hierarchical Structure Toward High Performance Supercapacitor Electrodes.

Supercapacitors (SCs) with outstanding versatility have a lot of potential applications in next-generation electronics. However, their practical uses are limited by their short working potential window and ultralow-specific capacity. Herein, the facile one-step in-situ hydrothermal synthesis is employed for the construction of a NiMo3S4/BP (black phosphorous) hybrid with a 3D hierarchical structure. After optimization, the NiMo3S4/BP hybrid displays a high specific capacitance of 830 F/g at 1 A/g compared to the pristine NiMo3S4 electrode. The fabricated NiMo3S4/BP//NiCo2S4/Ti3C2Tx asymmetric supercapacitor exhibits a better specific capacitance of 120 F/g at 0.5 A/g, which also demonstrates a high energy density of 54 Wh/kg at 1148.53 W/kg and good cycle stability with capacity retention of 86% and 97% of Coulombic efficiency after 6000 cycles. Further from the DFT simulations, the hybrid NiMo3S4/BP structure shows higher conductivity and quantum capacitance, which demonstrate greater charge storage capability, due to enhanced electronic states near the Fermi level. The lower diffusion energy barrier for the electrolyte K+ ions in the hybrid structure is facilitated by improved charge transfer performance for the hybrid NiMo3S4/BP. This work highlights the potential significance of hybrid nanoarchitectonics and compositional tunability as an emerging method for improving the charge storage capabilities of active electrodes.

Preparation of carbon-coated Fe2 O3 @Ti3 C2 Tx composites by mussel-like modifications as high-performance anodes for lithium-ion batteries.

Fe2 O3 with high theoretical capacity (1007 mA h g-1 ) and low cost is a potential anode material for lithium-ion batteries (LIBs), but its practical application is restricted by its low electrical conductivity and large volume changes during lithiation/delithiation. To solve these problems, Fe2 O3 @Ti3 C2 Tx composites were synthesized by a mussel-like modification method, which relies on the self-polymerization of dopamine under mild conditions. During polymerization, the electronegative group (-OH) on dopamine can easily coordinate with Fe3+ ions as well as form hydrogen bonds with the -OH terminal group on the surface of Ti3 C2 Tx , which induces a uniform distribution of Fe2 O3 on the Ti3 C2 Tx surface and mitigates self-accumulation of MXene nanosheets. In addition, the polydopamine-derived carbon layer protects Ti3 C2 Tx from oxidation during the hydrothermal process, which can further improve the electrical conductivity of the composites and buffer the volume expansion and particle agglomeration of Fe2 O3 . As a result, Fe2 O3 @Ti3 C2 Tx anodes exhibit ~100 % capacity retention with almost no capacity loss at 0.5 A g-1 after 250 cycles, and a stable capacity of 430 mA h g-1 at 2 A g-1 after 500 cycles. The unique structural design of this work provides new ideas for the development of MXene-based composites in energy storage applications.

Why do Single-Atom Alloys Catalysts Outperform both Single-Atom Catalysts and Nanocatalysts on MXene?

Single-atom alloys (SAAs), combining the advantages of single-atom and nanoparticles (NPs), play an extremely significant role in the field of heterogeneous catalysis. Nevertheless, understanding the catalytic mechanism of SAAs in catalysis reactions remains a challenge compared with single atoms and NPs. Herein, ruthenium-nickel SAAs (RuNiSAAs ) synthesized by embedding atomically dispersed Ru in Ni NPs are anchored on two-dimensional Ti3 C2 Tx MXene. The RuNiSAA-3 -Ti3 C2 Tx catalysts exhibit unprecedented activity for hydrogen evolution from ammonia borane (AB, NH3 BH3 ) hydrolysis with a mass-specific activity (rmass ) value of 333 L min-1 gRu -1 . Theoretical calculations reveal that the anchoring of SAAs on Ti3 C2 Tx optimizes the dissociation of AB and H2 O as well as the binding ability of H* intermediates during AB hydrolysis due to the d-band structural modulation caused by the alloying effect and metal-supports interactions (MSI) compared with single atoms and NPs. This work provides useful design principles for developing and optimizing efficient hydrogen-related catalysts and demonstrates the advantages of SAAs over NPs and single atoms in energy catalysis.

Swelling of Ti3 C2 Tx MXene in Water and Methanol at Extreme Pressure Conditions.

Pressure-induced swelling has been reported earlier for several hydrophilic layered materials. MXene Ti3C2Tx is also a hydrophilic layered material composed by 2D sheets but so far pressure-induced swelling is reported for this material only under conditions of shear stress at MPa pressures. Here, high-pressure experiments are performed with MXenes prepared by two methods known to provide "clay-like" materials. MXene synthesized by etching MAX phase with HCl+LiF demonstrates the effect of pressure-induced swelling at 0.2GPa with the insertion of additional water layer. The transition is incomplete with two swollen phases (ambient with d(001) = 16.7Å and pressure-induced with d(001) = 19.2Å at 0.2GPa) co-existing up to the pressure point of water solidification. Therefore, the swelling transition corresponds to change from two-layer water intercalation (2L-phase) to a never previously observed three-layer water intercalation (3L-phase) of MXene. Experiments with MXene prepared by LiCl+HF etching have not revealed pressure-induced swelling in liquid water. Both MXenes also show no anomalous compressibility in liquid methanol. The presence of pressure-induced swelling only in one of the MXenes indicates that the HCl+LiF synthesis method is likely to result in higher abundance of hydrophilic functional groups terminating 2D titanium carbide.

Functionalized MXene Films with Substantially Improved Low-Voltage Actuation.

Ti3 C2 Tx MXene film is promising for low-voltage electrochemical actuators (ECAs) due to its excellent electrical conductivity, volumetric capacitance, and mechanical properties. However, its in-plane actuation is limited to little intralayer strain of MXene sheets under polarization. Here it is demonstrated that a simple tetrabutylammonium (TBA) functionalization of MXene improves the in-plane actuation strain by 337% and also enhances the mechanical property and stability in air and the electrolyte. Various in situ characterizations reveal that the improved actuation is ascribed to the co-insertion/desertion of TBA and Li ions into/from MXene interlayer galleries and inter-edge gaps that causes a large in-plane sliding of MXene sheets under negative/positive polarizations. The assembled bending actuator has a high strength and modulus and generates a peak-to-peak strain difference of 0.771% and a blocking force up to 51.5 times its own weight under 1V. The designed soft robotic tweezer can grasp an object under 1V and hold it firmly under 0V. The novel sheet sliding mechanism resembling the filament sliding theory in skeletal muscles may inspire the design of high-performance actuators with other nanomaterials.

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 0.05-250ng/mL with an acceptable correlation coefficient (R2 ≥0.9984) and detection limits of 0.010-0.015ng/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.

Stepless IR Chromism in Ti3 C2 Tx MXene Tuned by Interlayer Water Molecules.

Real-time control over infrared (IR) radiation of objects is highly desired in a variety of areas such as personal thermal regulation and IR camouflage. This requires the dynamic modulation of IR emissivity in a stepless manner over a wide range (>50%), which remains a daunting challenge. Here, an emissivity modulation phenomenon is reported in stacked 2D Ti3 C2 Tx MXene nanosheets, from 12% to 68% as the intercalation/discharging of water molecules within the interlayers. The intercalation of water molecules dynamically changes the electronic properties and the complex permittivity in IR frequencies of Ti3 C2 Tx . This emissivity modulation is a stepless and reversible process without the assistance of any external energy input. Further, intercalating cellulose nanofibers into the Ti3 C2 Tx interlayers makes this dynamic process highly repeatable. Last, a sweat-responsive adaptive textile that can improve thermal comfort of human body under changes in metabolic rates and environmental conditions is demonstrated, showing great potential of this mechanism in passive on-demand radiation modulation.

Interface Engineering to Drive High-Performance MXene/PbS Quantum Dot NIR Photodiode.

The realization of a controllable transparent conducting system with selective light transparency is crucial for exploring many of the most intriguing effects in top-illuminated optoelectronic devices. However, the performance is limited by insufficient electrical conductivity, low work function, and vulnerable interface of traditional transparent conducting materials, such as tin-doped indium oxide. Here, it is reported that two-dimensional (2D)titanium carbide (Ti3 C2 Tx ) MXene film acts as an efficient transparent conducting electrode for the lead sulfide (PbS) colloidal quantum dots (CQDs) photodiode with controllable near infrared transmittance. The solution-processed interface engineering of MXene and PbS layers remarkably reduces the interface defects of MXene/PbS CQDs and the carrier concentration in the PbS layer. The stable Ti3 C2 Tx /PbS CQDs photodiodes give rise to a high specific detectivity of 5.51×1012 cmW-1 Hz1/2 , a large dynamic response range of 140dB, and a large bandwidth of 0.76MHz at 940nm in the self-powered state, ranking among the most exceptional in terms of comprehensive performance among reported PbS CQDs photodiodes. In contrast with the traditional photodiode technologies, this efficient and stable approach opens a new horizon to construct widely used infrared photodiodes with CQDs and MXenes.

Near-Atomic-Scale Perspective on the Oxidation of Ti3 C2 Tx MXenes: Insights from Atom Probe Tomography.

MXenes are a family of 2D transition metal carbides and nitrides with remarkable properties, bearing great potential for energy storage and catalysis applications. However, their oxidation behavior is not yet fully understood, and there are still open questions regarding the spatial distribution and precise quantification of surface terminations, intercalated ions, and possible uncontrolled impurities incorporated during synthesis and processing. Here, atom probe tomography (APT) analysis of as-synthesized Ti3 C2 Tx MXenes reveals the presence of alkali (Li, Na) and halogen (Cl, F) elements as well as unetched Al. Following oxidation of the colloidal solution of MXenes, it is observed that the alkalis are enriched in TiO2 nanowires. Although these elements are tolerated through the incorporation by wet chemical synthesis, they are often overlooked when the activity of these materials is considered, particularly during catalytic testing. This work demonstrates how the capability of APT to image these elements in 3D at the near-atomic scale can help to better understand the activity and degradation of MXenes, in order to guide their synthesis for superior functionalproperties.

Asymmetric Supercapacitors based on 1,10-phenanthroline-5,6-dione Molecular Electrodes Paired with MXene.

An efficient approach to increase the energy density of supercapacitors is to prepare electrode materials with larger specific capacitance and increase the potential difference between the positive and negative electrodes in the device. Herein, an organic molecular electrode (OME) is prepared by anchoring 1,10-phenanthroline-5,6-dione (PD), which possesses two pyridine rings and an electron-deficient conjugated system, onto reduced graphene oxide (rGO). Because of the electron-deficient conjugated structure of PD molecule, PD/rGOs exhibit a more positive redox peak potential along with the advantages of high capacitance-controlled behaviour and fast reaction kinetics. Additionally, the small energy gap between the lowest unoccupied molecular orbital (LUMO) and highest occupied molecular orbital (HOMO) leads to increased conductivity in PD/rGO. To assemble the asymmetric supercapacitor (ASC), a two-dimensional metal carbide, as known as MXene, with a chemical composition of Ti3C2Tx is selected as the negative electrode due to its exceptional performance, and PD/rGO-0.5 is employed as the positive electrode. Consequently, the working voltage is expanded up to 1.8 V. Through further electrochemical measurements, the assembled ASC (PD/rGO-0.5//Ti3C2Tx) achieves a remarkable energy density of 36.8 Wh kg-1. Remarkably, connecting two ASCs in series can power 73 LEDs, showcasing its promising potential for energy storage applications.

MXene-Integrated Perylene Anode with Ultra-Stable and Fast Ammonium-Ion Storage for Aqueous Micro Batteries.

The aqueous micro batteries (AMBs) are expected to be one of the most promising micro energy storage devices for its safe operation and cost-effectiveness. However, the performance of the AMBs is not satisfactory, which is attributed to strong interaction between metal ions and the electrode materials. Here, the first AMBs are developed with NH4 + as charge carrier. More importantly, to solve the low conductivity and the dissolution during the NH4 + intercalation/extraction problem of perylene material represented by perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA), the Ti3 C2 Tx MXene with high conductivity and polar surface terminals is introduced as a conductive skeleton (PTCDA/Ti3 C2 Tx MXene). Benefitting from this, the PTCDA/Ti3 C2 Tx MXene electrodes exhibit ultra-high cycle life and rate capability (74.31% after 10000 galvanostatic chargedischarge (GCD) cycles, and 91.67 mAh g-1 at 15.0 A g-1 , i.e., capacity retention of 45.2% for a 30-fold increase in current density). More significantly, the AMBs with NH4 + as charge carrier and PTCDA/Ti3 C2 Tx MXene anode provide excellent energy density and power density, cycle life, and flexibility. This work will provide strategy for the development of NH4 + storage materials and the design of AMBs.

Flexible Ti3 C2 Tx MXene Bonded Bio-Derived Carbon Fibers Support Tin Disulfide for Fast and Stable Sodium Storage.

High energy density and flexible electrodes, which have high mechanical properties and electrochemical stability, are critical to the development of wearable electronics. In this work, a free-standing MXene bonded SnS2 composited nitrogen-doped carbon fibers (MXene/SnS2 @NCFs)film is reported as a flexible anode for sodium-ion batteries. SnS2 nanoparticles with high-capacity properties are covalently decorated in bio-derived nitrogen-doped 1D carbon fibers (SnS2 @NCFs) and further assembled with highly conductive MXene sheets. The addition of bacterial cellulose (BC) can further improve the flexibility of the film. The unique 3D structure of points, lines, and planes can not only offset the disadvantage of low conductivity of SnS2 nanoparticles but also expand the distance between MXene sheets, which is conducive to the penetration of electrolytes. More importantly, the MXene sheets and N-doped 1D carbon fibers (NCFs) can accommodate the large volume expansion of SnS2 nanoparticles and trap polysulfide during the cycle. The MXene/SnS2 @NCFs film exhibits better sodium storage and excellent rate performance compared to the SnS2 @NCFs. The in situ XRD and ex situ (XRD, XPS, and HRTEM) techniques are used to analyze the sodiation process and to deeply study the reaction mechanism of the films. Finally, the quasi-solid-state full cells with MXene/SnS2 @NCFs and Na3 V2 (PO4 )3 @carbon cloth (NVP@CC) fully demonstrate the application potential of the flexible electrodes.

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 3nm in a solution of NMP and NBA; it shows a direct bandgap semiconductor with a bandgap of 3eV and a specific capacitance of 41Fg-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 524Fg-1 at 1Ag-1 in 6m H2 SO4 electrolyte, a high capacity retention of 75%, and a minimum relaxation time of 0.51s. 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 552mFcm-2 at 1.25mAcm-2 , a retention rate of 75%, a capacity retention of 93% after 5000 cycles, and an energy density of 40.4Whcm-3 at a volume power density of 416Wcm-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.

Inorganic-Organic Nanoarchitectonics: MXene/Covalent Organic Framework Heterostructure for Superior Microextraction.

One of the difficulties limiting covalent organic frameworks (COFs) from becoming excellent adsorbents is their stacking/aggregation architectures owing to poor morphology/structure control during the synthesis process. Herein, an inorganic-organic nanoarchitectonics strategy to synthesize the MXene/COF heterostructure (Ti3 C2 Tx /TAPT-TFP) is developed by the assembly of β-ketoenamine-linked COF on the Ti3 C2 Tx MXene nanosheets. The as-prepared Ti3 C2 Tx /TAPT-TFP retains the 2D architecture and high adsorption capacity of MXenes as well as large specific surface area and hierarchical porous structureof COFs. As a proof of concept, the potential of Ti3 C2 Tx /TAPT-TFP for solid-phase microextraction (SPME) of trace organochlorine pesticides (OCPs)is investigated. The Ti3 C2 Tx /TAPT-TFP based SPME method achieves low limits of detection (0.036-0.126ngg-1 ), wide linearity ranges (0.12-20.0ngg-1 ), and acceptable repeatabilities for preconcentrating trace OCPs from fruit and vegetable samples. This study offers insights into the potential of constructing COF or MXene-based heterostructures for the microextraction of environmental pollutants.

Powering the Future: Unleashing the Potential of MXene-Based Dual-Functional Photoactive Cathodes in Photo-Rechargeable Zinc-Ion Capacitor.

Dual-functional photo-rechargeable (photo-R) energy storage devices, which acquire stored energy from solar energy harvesting, are being developed to battle the current energy crisis. In this study, these findings on the photo-driven characteristics of MXene-based photocathodes in photo-R zinc-ion capacitors (ZICs) are presented. Along with the pristine Ti3 C2 Tx MXene, tellurium/Ti3 C2 Tx (Te/Ti3 C2 Tx ) hybrid nanostructure is synthesized via facile chemical vapor transport technique to examine them for photocathodes in ZICs. Interestingly, the evaluated self-powered photodetector devices using MXene-based samples revealed a pyro-phototronic behavior introduced into the samples, with higher desirability observed in Te/Ti3 C2 Tx . The photo-R ZICs results exhibited a capacitance enhancement of 50.86% for Te/Ti3 C2 Tx at two scan rates of 5 and 10mVs-1 under illumination, compared to dark conditions. In contrast, a capacitance enhancement of 30.20% is obtained for the pristine Ti3 C2 Tx at only a 5mVs-1 scan rate. Furthermore, both samples achieved photo-charging voltage responses of ≈960mV, and photoconversion efficiencies of 0.01% (for Te/ Ti3 C2 Tx ) and 0.07% (for Ti3 C2 Tx ). These characteristics in MXene-based single photo-R ZICs are significant and considerable with the distinguished integrated photo-R supercapacitors with solar cells, or coupled energy-harvesting and energy-storing devices reported recently in the literature.

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.

Operando Spectroscopy Observation of Mo Clusters-Ti3 C2 TX Catalyst/Support Interface's Dynamic Evolution in Hydrogen Evolution Reaction.

The interaction between catalyst and support plays an important role in electrocatalytic hydrogen evolution (HER), which may explain the improvement in performance by phase transition or structural remodeling. However, the intrinsic behavior of these catalysts (dynamic evolution of the interface under bias, structural/morphological transformation, stability) has not been clearly monitored, while the operando technology does well in capturing the dynamic changes in the reaction process in real time to determine the actual active site. In this paper, nitrogen-doped molybdenumatom-clusters on Ti3 C2 TX (MoACs /N-Ti3 C2 TX ) is used as a model catalyst to reveal the dynamic evolution of MoAcs on Ti3 C2 TX during the HER process. Operando X-ray absorption structure (XAS) theoretical calculation and in situ Raman spectroscopy showed that the Mo cluster structure evolves to a 6-coordinated monatomic Mo structure under working conditions, exposing more active sites and thus improving the catalytic performance. It shows excellent HER performance comparable to that of commercial Pt/C, including an overpotential of 60mV at 10mA cm-2 , a small Tafel slope (56mV dec-1 ), and high activity and durability. This study provides a unique perspective for investigating the evolution of species, interfacial migration mechanisms, and sources of activity-enhancing compounds in the process of electroreduction.