Tetrabutylammonium Bromide Functionalized Ti3C2Tx MXene as Versatile Cathode Buffer Layer for Efficient and Stable Inverted Perovskite Solar Cells

2D Ti₃C₂T_x MXene, possessing facile preparation, high electrical conductivity, flexibility, and solution processability, shows good application potential for enhancing device performance of perovskite solar cells (PVSCs). In this study, tetrabutylammonium bromide functionalized Ti₃C₂T_x (TBAB-Ti₃C₂T_x) is developed as cathode buffer layer (CBL) to regulate the PCBM/Ag cathode interfacial property for the first time. By virtue of the charge transfer from TBAB to Ti₃C₂T_x demonstrated by electron paramagnetic resonance and density functional theory, the TBAB-Ti₃C₂T_x CBL with high electrical conductivity exhibits significantly reduced work function of 3.9 eV, which enables optimization of energy level alignment and enhancement of charge extraction. Moreover, the TBAB-Ti₃C₂T_x CBL can effectively inhibit the migration of iodine ions from perovskite layer to Ag cathode, which synergistically suppresses defect states and reduce charge recombination. Consequently, utilizing MAPbI₃ perovskite without post-treatment, the TBAB-Ti₃C₂T_x based device exhibits a dramatically improved power conversion efficiency of 21.65% with significantly improved operational stability, which is one of the best efficiencies reported for the devices based on MAPbI₃/PCBM with different CBLs. These results indicate that TBAB-Ti₃C₂T_x shall be a promising CBL for high-performance inverted PVSCs and inspire the further applications of quaternary ammonium functionalized MXenes in PVSCs.     

Atomic Sulfur Covalently Engineered Interlayers of Ti3C2 MXene for Ultra‐Fast Sodium‐Ion Storage by Enhanced Pseudocapacitance

2D MXenes have been widely applied in the field of electrochemical energy storage owning to their high electrical conductivity and large redox‐active surface area. However, electrodes made from multilayered MXene with small interlayer spacing exhibit sluggish kinetics with low capacity for sodium‐ion storage. Herein, Ti₃C₂ MXene with expanded and engineered interlayer spacing for excellent storage capability is demonstrated. After cetyltrimethylammonium bromide pretreatment, S atoms are successfully intercalated into the interlayer of Ti₃C₂ to form a desirable interlayer‐expanded structure via Ti? S bonding, while pristine Ti₃C₂ is hardly to be intercalated. When the annealing temperature is 450 °C, the S atoms intercalated Ti₃C₂ (CT‐S@Ti₃C₂‐450) electrode delivers the improved Na‐ion capacity of 550 mAh g^?1 at 0.1 A g^?1 (≈120 mAh g^?1 at 15 A g^?1, the best MXene‐based Na⁺‐storage rate performance reported so far), and excellent cycling stability over 5000 cycles at 10 A g^?1 by enhanced pseudocapacitance. The enhanced sodium‐ion storage capability has also been verified by theoretical calculations and kinetic analysis. Coupling the CT‐S@Ti₃C₂‐450 anode with commercial AC cathode, the assembled Na⁺ capacitor delivers high energy density (263.2 Wh kg^?1) under high power density (8240 W kg^?1), and outstanding cycling performance.     

Tailoring Ultrahigh Energy Density and Stable Dendrite-Free Flexible Anode with Ti3C2Tx MXene Nanosheets and Hydrated Ammonium Vanadate Nanobelts for Aqueous Rocking-Chair Zinc Ion Batteries

Exploiting Zn metal-free anode materials would be an effective strategy to resolve the problems of Zn metal dendrites that severely hinder the development of Zn ion batteries (ZIBs). However, the study of Zn metal-free anode materials is still in their infancy, and more importantly, the low energy density severely limits their practical implementations. Herein, a novel (NH₄)₂V₁₀O₂₅ · 8H₂O@Ti₃C₂T_x (NHVO@Ti₃C₂T_x) film anode is proposed and investigated for constructing “rocking-chair” ZIBs. The NHVO@Ti₃C₂T_x electrode shows a capacity of 514.7 mAh g⁻¹ and presents low potential which is 0.59 V (vs Zn²⁺/Zn) at 0.1 A g⁻¹. The introduction of Ti₃C₂T_x not only affords an interconnected conductive network, but also stabilizes the NHVO nanobelts structure for a long cycle life (84.2% retention at 5.0 A g⁻¹ over 6000 cycles). As a proof-of-concept, a zinc metal-free full battery is successfully demonstrated, which delivers the highest capacity of 131.7 mAh g⁻¹ (mass containing anodic and cathodic) and energy density of 97.1 Wh kg⁻¹ compared to all reported aqueous “rocking-chair” ZIBs. Furthermore, a long cycling span of 6000 cycles is obtained with capacity retention reaching up to 92.1%, which is impressive. This work is expected to provide new moment toward V-based materials for “rocking-chair” ZIBs.     

Smart Energy Bricks: Ti3C2@Polymer Electrochemical Energy Storage inside Bricks by 3D Printing

Three-dimensional (3D) printing technology has a pronounced impact on building construction and energy storage devices. Here, the concept of integrating 3D-printed electrochemical devices into insulation voids in construction bricks is demonstrated in order to create electrochemical energy storage as an integral part of home building. The low-cost 3D-printed supercapacitor (SC) electrodes are created using graphene/polylactic acid (PLA) filament in any desired shape such as 3D cylindrical- (3Dcy), disk- (3Ddc), and 3D rectangular- (3Drc) shaped electrodes. To obtain excellent capacitive performance, a Ti₃C₂@polypyrrole (PPy) hybrid is uniformly electroplated on the surface of 3D-printed electrodes. These Ti₃C₂@PPy-coated 3D-printed electrodes exhibit outstanding electrical conductivity, capacitive performance, cycle life, and power density. The bricks themselves act as an excellent scaffold for electrochemical energy devices as they are electrically insulating, fire-resistant, and contain substantial unused thermal insulation voids. A 3Drc Ti₃C₂@PPy SC is integrated into a real brick to showcase a smart house energy storage system that allows to reserve power in the bricks and use it as a power backup source in the event of a power outage in the elevator. This concept provides a platform for future truly smart buildings built from added value “smart brick” energy storage systems.     

Controllable Patterning of Porous MXene (Ti3C2) by Metal-Assisted Electro-Gelation Method

Since discovered in 2011, transition metal carbides or nitrides (MXenes) have attracted enormous attention due to their unique properties. Morphology regulation strategies assembling 2D MXene sheets into 3D architecture have endowed the as-formed porous MXene with a better performance in various fields. However, the direct patterning strategy for the porous MXene into integration with multifunctional and multichannel electronic devices still needs to be investigated. The metal-assisted electro-gelation method the authors propose can directly generate porous-structured MXene hydrogel with a tunable feature. By electrolyzing the sacrificial metal, the released metal cations initiate the electro-gelation process during which electrostatic interactions occur between cations and the MXene sheets. A high spatial resolution down to micro-meter level is achieved utilizing the method, enabling high-performance hydrogels with more complex architectures. Electronics prepared through this metal-assisted electro-gelation process have shown promising applications of the porous MXene in energy and biochemical sensing fields. Energy storage devices with a capacitance at 33.3 mF cm⁻² and biochemical sensors show prominent current responses towards metabolites (sensitivity of H₂O₂: 165.6  µ A mm ⁻¹ cm⁻²; sensitivity of DA: 212 nA  µ m ⁻¹ cm⁻²), suggesting that the metal-assisted electro-gelation method will become a prospective technique for advanced fabrication of MXene-based devices.     

High-Performance Ultraviolet Photodetectors Enabled by van der Waals Schottky Junction Based on TiO2 Nanorod Arrays/Au-Modulated Ti3C2Tx MXene

Two-dimensional transition metal carbides and nitrides (MXenes) show tremendous potential for optoelectronic devices due to their excellent electronic properties. Here, a high-performance ultraviolet photodetector based on TiO₂ nanorod arrays/Ti₃C₂T_x MXene van der Waals (vdW) Schottky junction by all-solution process technique is reported. The Ti₃C₂T_x MXene modulated by the Au electrode increases its work function from 4.41 to 5.14 eV to form a hole transport layer. Complemented by the dangling bond-free surface of Ti₃C₂T_x, the Fermi-level pinning effect is suppressed and the electric-field strength of the Schottky junction is enhanced, which promotes charge separation and transport. After applying a bias of −1.5 V, the photovoltaic effect is favorably reinforced, while the hole-trapping mechanism (between TiO₂ and oxygen) and reverse pyroelectric effect are largely eliminated. As a result, the responsivity and specific detectivity of the device with FTO/TiO₂ nanorod arrays/Ti₃C₂T_x/Au structure reach 1.95 × 10⁵ mA W⁻¹ and 4.3 × 10¹³ cm Hz^1/2 W⁻¹ (370 nm, 65 mW cm⁻²), respectively. This work provides an effective approach to enhance the performance of photodetectors by forming the vdW Schottky junction and choosing metal electrodes to modulate MXene as a suitable charge transport layer.     

Surface‐Modified Metallic Ti3C2Tx MXene as Electron Transport Layer for Planar Heterojunction Perovskite Solar Cells

MXenes are a large and rapidly expanding family of 2D materials that, owing to their unique optoelectronic properties and tunable surface termination, find a wide range of applications including energy storage and energy conversion. In this work, Ti₃C₂T_x MXene nanosheets are applied as a novel type of electron transport layer (ETL) in low‐temperature processed planar‐structured perovskite solar cells (PSCs). Interestingly, simple UV‐ozone treatment of the metallic Ti₃C₂T_x that increases the surface Ti? O bonds without any change in its bulk properties such as high electron mobility improves its suitability as an ETL. Improved electron transfer and suppressed recombination at the ETL/perovskite interface results in augmentation of the power conversion efficiency (PCE) from 5.00% in the case of Ti₃C₂T_x without UV‐ozone treatment to the champion PCE of 17.17%, achieved using the Ti₃C₂T_x film after 30 min of UV‐ozone treatment. As the first report on the use of pure MXene layer as an ETL in PSCs, this work shows the great potential of MXenes to be used in PSCs and displays their promise for applications in photovoltaic technology in general.     

Tuning Thermal Transport Through Atomically Thin Ti3C2Tz MXene by Current Annealing in Vacuum

Heat transport across vertical interfaces of heterogeneous 2D materials is usually governed by the weak Van der Waals interactions of the surface‐terminating atoms. Such interactions play a significant role in thermal transport across transition metal carbide and nitride (MXene) atomic layers due to their hydrophilic nature and variations in surface terminations. Here, the metallicity of atomically thin Ti₃C₂T_z MXene, which is also verified by scanning tunneling spectroscopy for the first time, is exploited to develop a self‐heating/self‐sensing platform to carry out direct‐current annealing experiments in high (<10^?8 bar) vacuum, while simultaneously evaluating the interfacial heat transport across a Ti₃C₂T_z/SiO₂ interface. At room temperature, the thermal boundary conductance (TBC) of this interface is found, on average, to increase from 10 to 27 MW m^?2 K^?1 upon current annealing up to the breakdown limit. In situ heating X‐ray diffraction and X‐ray photo‐electron spectroscopy reveal that the TBC values are mainly affected by interlayer and interface spacing due to the removal of absorbents, while the effect of surface termination is negligible. This study provides key insights into understanding energy transport in MXene nanostructures and other 2D material systems.     

Strategy Toward Semiconducting Ti3C2Tx-MXene: Phenylsulfonic Acid Groups Modified Ti3C2Tx as Photosensitive Material for Flexible Visual Sensory-Neuromorphic System

The excellent electronic and electrochemical properties make 2D MXenes suitable candidates for sensors, batteries, and supercapacitors. However, the metallic-like behavior of MXenes hinders their potential for optoelectronic devices such as photodetectors. In this study, the band gap of metalloid Ti₃C₂T_x MXene is successfully opened to 1.53 eV with phenylsulfonic acid groups and realized a transistor and high-performance near-infrared photodetector array for a flexible vision sensory-neuromorphic system. The phenylsulfonic acid groups modified Ti₃C₂T_x MXene (S-Ti₃C₂T_x)-based flexible photodetector has a maximum responsivity of 8.50×10² A W⁻¹ and a detectivity of 3.69×10¹¹ Jones under 1064 nm laser irradiation. Moreover, the fabricated flexible vision sensory-neuromorphic system for image recognition realizes a high recognition rate >0.99, leading to great potential in the field of biological visual simulation and biomimetic eye. Besides conventional devices with Au as the conductive electrodes, all Ti₃C₂T_x MXene-based devices are also fabricated with S-Ti₃C₂T_x as the photosensitive material and unmodified Ti₃C₂T_x as the conductive electrodes, exhibiting comparable optoelectronic performances.     

Removal of Interlayer Water of two Ti3C2Tx MXenes as a Versatile Tool for Controlling the Fermi-Level Pinning-Free Schottky Diodes with Nb:SrTiO3

Striving for the sixth-generation communication technology discovery, semiconductors beyond Si with wider bandgaps as well as non-conventional metals are actively being sought to achieve high speeds whilst maintaining devices miniaturization. 2D materials may provide the potential for downsizing, but their functional advantage over existing counterparts still longs to be discovered. Along that path, surface-adsorbed or bulk-intercalated water molecules remaining after wet-chemical synthesis of 2D materials are generally seen as obstacles to high-performance achievement. Herein, the control of such water within the interlayers of solution-processed metallic 2D titanium carbide (MXene) by vacuum annealing duration is demonstrated. Moreover, the impact of water removal on work function (WF) and functional terminations is unveiled for the first time. Furthermore, the usefulness of such water for controlling a novel Schottky diode in contact with an n-type oxide semiconductor, niobium-doped strontium titanate (Nb:SrTiO₃) is observed. The advantage of MXene compared to conventional gold as facile processing, WF tunability, and lower turn-on voltage in the Schottky anode application is highlighted. This fundamental study shows the way for a novel Schottky diode preparation in atmospheric conditions and provides implications for further research directions aiming at commercialization.     

High Linearity,Low Hysteresis Ti3C2Tx MXene/AgNW/Liquid Metal Self-Healing Strain Sensor Modulated by Dynamic Disulfide and Hydrogen Bonds

Flexible wearable strain sensors have received extensive attention in human–computer interaction, soft robotics, and human health monitoring. Despite significant efforts in developing stretchable electronic materials and structures, developing flexible strain sensors with stable interfaces and low hysteresis remains a challenge. Herein, Ti₃C₂T_x MXene/AgNWs/liquid metal strain sensors (MAL strain sensor) with self-healing function are developed by exploiting the strong interactions between Ti₃C₂T_x MXene/AgNWs/LM and the disulfide and hydrogen bonds inside the self-healing poly(dimethylsiloxane) elastomers. AgNWs lap the Ti₃C₂T_x MXene sheets, and the LM acts as a bridge to increase the lap between Ti₃C₂T_x MXene and AgNWs, thereby improving the interface interaction between them and reducing hysteresis. The MAL strain sensor can simultaneously achieve high sensitivity (gauge factor for up to 3.22), high linearity (R² = 0.98157), a wide range of detection (e.g., 1%–300%), a fast response time (145 ms), excellent repeatability, and stability.In addition, the MAL strain sensor before and after self-healing is combined with a small fish and an electrothermally driven soft robot, respectively, allowing real-time monitoring of the swinging tail of the small fish and the crawling of the soft robot by resistance changes.     

Intercalation of Metal Ions into Ti3C2Tx MXene Electrodes for High‐Areal‐Capacitance Microsupercapacitors with Neutral Multivalent Electrolytes

Microsupercapacitors (MSCs) with neutral multivalent electrolytes are safer, cheaper, and exhibit higher theoretical energy densities compared with the MSCs with acidic and alkaline electrolytes. Multivalent charge carriers (e.g., Mg²⁺, Zn²⁺) in the MSCs with Ti₃C₂T_x MXene electrodes have not been demonstrated, which could theoretically achieve higher specific capacitances and energy densities. However, because of the larger size of multivalent charge carriers, the MXene electrodes require further modifications to facilitate reversible electrochemical reactions. Herein, through spontaneous intercalation of various metal ions into MXene multilayers, twelve metal ion intercalated MXene electrodes (Mⁿ⁺‐MXene) are fabricated and demonstrate improved electrochemical performance. Different nanopillar effects are observed between divalent Be²⁺ and trivalent Al³⁺ intercalants, which are systematically investigated by electrochemical impedance spectroscopy and molecular dynamics simulation. Among all Mⁿ⁺‐MXene electrodes, the Be²⁺‐MXene electrode largely facilitates the charge‐transfer process with minimal disturbance of electrolyte diffusion rates, showing improved specific capacitances and high rate performance in univalent (Li₂SO₄, Na₂SO₄, K₂SO₄) and multivalent electrolytes (BeSO₄, MgSO₄, ZnSO₄). Finally, flexible Be²⁺‐MXene MSCs with neural ZnSO₄ gel electrolytes are fabricated, demonstrating superior areal capacitances (77.2 mF cm^?2) and high energy density (3.86 μWh cm^?2 at 0.12 mW cm^?2) together with high user safety.     

Full-Temperature All-Solid-State Ti3C2Tx/Aramid Fiber Supercapacitor with Optimal Balance of Capacitive Performance and Flexibility

Full-temperature all-solid-state flexible symmetrical fiber supercapacitors (FSCs) are assembled by using montmorillonite flake/polyvinyl alcohol organic hydrogel (F-MMT/PVA OHGE) as the electrolyte and separator and Ti₃C₂T_x/ANF-5% (T/A-5) fiber as the electrode, in which T/A-5 fiber is prepared by using delaminated Ti₃C₂T_x nanosheets as assembled units and 5% of aramid nanofiber (ANF) as the functional additive using a wet spinning method in a coagulated bath with 0.5 m FeCl₂ solution. The T/A-5 hybrid fiber exhibits a specific capacity of 807 F cm⁻³ in 3 m H₂SO₄ electrolyte, a superior mechanical strength of 104 MPa, and a high conductivity of 1025 S cm⁻¹. The assembled F-MMT/PVA OHGE T/A-5 FSC not only shows a specific capacitance of 295 F cm⁻³ and a capacitance retention of 91% at a current density of 5 A cm⁻³ after 10 000 charging/discharging cycles, but also a maximum volumetric energy density of 26.2 mWh cm⁻³. Meanwhile, the assembled device displays good flexibility and excellent capacitance in a wide temperature range of −40 to 80 °C, the electrochemical performance of the FSC is maintained under varying degrees of bending. This study provides an effective strategy for designing and assembling of full-temperature all-solid-state symmetrical flexible FSCs with the optimal balance of capacitive performance and flexibility.     

Noble Metal Ion-Directed Assembly of 2D Materials for Heterostructured Catalysts and Metallic Micro-Texturing

Assembling 2D-material (2DM) nanosheets into micro- and macro-architectures with augmented functionalities requires effective strategies to overcome nanosheet restacking. Conventional assembly approaches involve external binders and/or functionalization, which inevitably sacrifice 2DM's nanoscale properties. Noble metal ions (NMI) are promising ionic crosslinkers, which can simultaneously assemble 2DM nanosheets and induce synergistic properties. Herein, a collection of NMI–2DM complexes are screened and categorized into two sub-groups. Based on the zeta potentials, two assembly approaches are developed to obtain 1) NMI-crosslinked 2DM hydrogels/aerogels for heterostructured catalysts and 2) NMI–2DM inks for templated synthesis. First, tetraammineplatinum(II) nitrate (TPtN) serves as an efficient ionic crosslinker to agglomerate various 2DM dispersions. By utilizing micro-textured assembly platforms, various TPtN–2DM hydrogels are fabricated in a scalable fashion. Afterward, these hydrogels are lyophilized and thermally reduced to synthesize Pt-decorated 2DM aerogels (Pt@2DM). The Pt@2DM heterostructures demonstrate high, substrate-dependent catalytic activities and promote different reaction pathways in the hydrogenation of 3-nitrostyrene. Second, PtCl₄ can be incorporated into 2DM dispersions at high NMI molarities to prepare a series of PtCl₄–2DM inks with high colloidal stability. By adopting the PtCl₄–graphene oxide ink, various Pt micro-structures with replicated topographies are synthesized with accurate control of grain sizes and porosities.     

Strain Sensors with a High Sensitivity and a Wide Sensing Range Based on a Ti3C2Tx (MXene) Nanoparticle–Nanosheet Hybrid Network

A high sensitivity and large stretchability are desirable for strain sensors in wearable applications. However, these two performance indicators are contradictory, since the former requires a conspicuous structural change under a tiny strain, whereas the latter demands morphological integrity upon a large deformation. Developing strain sensors with both a high sensitivity (gauge factor (GF) > 100) and a broad strain range (>50%) is a considerable challenge. Herein, a unique Ti₃C₂T_x MXene nanoparticle–nanosheet hybrid network is constructed. The migration of nanoparticles leads to a large resistance variation while the wrapping of nanosheet bridges the detached nanoparticles to maintain the connectivity of the conductive pathways in a large strain region. The synergetic motion of nanoparticles and nanosheets endows the hybrid network with splendid electrical–mechanical performance, which is reflected in its high sensitivity (GF > 178.4) over the entire broad range (53%), the super low detection limit (0.025%), and a good cycling durability (over 5000 cycles). Such high performance endows the strain sensor with the capability for full‐range human motion detection.     

Flexible Ti3C2Tx@Al electrodes with Ultrahigh Areal Capacitance: In Situ Regulation of Interlayer Conductivity and Spacing

Although Ti₃C₂ MXene has shown great potential in energy storage field, poor conductivity and restacking between MXene flakes seriously hinders the maximization of its capacitance. Herein, a new strategy to solve the problems is developed. Gallery Al atoms in Ti₃AlC₂ are partially removed by simple hydrothermal etching to get Ti₃C₂T_x reserving appropriate Al interlayers (Ti₃C₂T_x@Al). Ti₃C₂T_x@Al keeps stable layered structure rather than isolated Ti₃C₂T_x flakes, which avoids flake restacking. The removal of partial Al frees up space for easy electrolyte infiltration while the reserved Al as “electron bridges” ensures high interlayer conductivity. As a result, the areal capacitance reaches up to 1087 mF cm^?2 at 1 mA cm^?2 and over 95% capacitance is maintained after 6000 cycles. The all‐solid‐state supercapacitor (ASSS) based on Ti₃C₂T_x@Al delivers a high capacitance of 242.3 mF cm^?2 at 1 mV s^?1 and exhibits stable performance at different bending states. Two ASSSs in tandem can light up a light‐emitting diode under the planar or wrapping around an arm. The established strategy provides a new avenue to improve capacitance performances of MXenes.     

In Situ Formation of Multiple Schottky Barriers in a Ti3C2 MXene Film and its Application in Highly Sensitive Gas Sensors

The main gas‐sensing mechanisms of 2D materials are surface charge transfer by analytes and Schottky barrier (SB) modulation at the interface between the metallic and semiconducting surfaces. In particular, dramatic differences in the gas‐sensing performances of 2D materials originate from SB modulation. However, SB sites typically exist only at the interface between the semiconducting channel material and the metal electrode. Herein, in situ formed multiple SBs in a single gas‐sensing channel are demonstrated, which are derived from the heterojunction of metallic Ti₃C₂ and semiconducting TiO₂. In stark contrast with previous techniques, edge‐oxidized Ti₃C₂ flakes are synthesized by solution oxidation, allowing the uniform formation of TiO₂ crystals on all flakes that comprise the gas sensing channel. Oxidized colloidal solutions are subjected to vacuum filtration to automatically form SB sites at the multiple inter‐flake junctions in both the outer surface and inner bulk regions of the film. The TiO₂/Ti₃C₂ composite sensor shows 13.7 times higher NO₂ sensitivity as compared with pristine Ti₃C₂ MXene, while the responses of the reducing gases are almost unchanged. The results suggest a new strategy for improving gas‐sensing performance by maximizing the density of SB sites through a simple method.     

3D HfO2 Thin Film MEMS Capacitor with Superior Energy Storage Properties

Capacitors are ubiquitous and crucial components in modern technologies. Future microelectronic devices require novel dielectric capacitors with higher energy storage density, higher efficiency, better frequency and temperature stabilities, and compatibility with integrated circuit (IC) processes. Here, in order to overcome these challenges, a novel 3D HfO₂ thin film capacitor is designed and fabricated by an integrated microelectromechanical system (MEMS) process. The energy storage density (ESD) of the capacitor reaches 28.94 J cm⁻³, and the energy storage efficiency of the capacitor is up to 91.3% under an applied electric field of 3.5 MV cm⁻¹. The ESD can be further improved by reducing the minimum period structure size of the 3D capacitor. Moreover, the 3D capacitor exhibits excellent temperature stability (up to 150 °C) and charge-discharge endurance (10⁷ cycles). The results indicate that the 3D HfO₂ thin film MEMS capacitor has enormous potential in energy storage applications in harsh environments, such as pulsed discharge and power conditioning electronics.     

Surface Energy Mediated Sulfur Vacancy of ZnIn2S4 Atomic Layers for Photocatalytic H2O2 Production

Constructing rich defect active site structure for material design is still a great challenge. Herein, a simple surface engineering strategy is demonstrated to construct one-unit-cell ZnIn₂S₄ atomic layers with the modulated surface energy of S vacancy. Rich surface energy can regulate and control the rich S vacancy, which ensures rich active sites, higher charge density and effective carrier transport. As a result, the ZnIn₂S₄ atomic layers with rich surface energy affords an obvious enhancement in H₂O₂ productive rate of 1592.04 µmol g⁻¹ h⁻¹, roughly 14.58 times superior to that with poor surface energy. Moreover, the in situ infrared diffuse reflection spectrum indicates that S vacancy as the oxygen reduction reaction active site is responsible for the critical intermediate *O₂⁻ and *OOH, corresponding to two-electron oxygen reduction reaction. This study provides a valuable insight and guidance for constructing controllably defects to achieve highly efficient H₂O₂ production.     

Mechanisms of the Planar Growth of Lithium Metal Enabled by the 2D Lattice Confinement from a Ti3C2Tx MXene Intermediate Layer

The propensity of Li to form irregular and nonplanar electrodeposits has become a fundamental barrier for fabricating Li metal batteries. Here, a planar, dendrite-free Li metal growth on 2D Ti₃C₂T_x MXene is reported. Ab initio calculations suggest that Li forms a hexagonal close-packed (hcp) layer on the surface of Ti₃C₂T_x via ionic bonding and the lattice confinement. The ionic bonding weakens gradually after a few monolayers, resulting in a nanometers-thin transition region of hcp-Li. Above this transition region, the deposition is dominated by plating of body-centered cubic (bcc) Li via metallic bonding. Formation of a dense and planar Li metal anode with preferential growth along the (110) facet is explained by the lattice matching between Ti₃C₂T_x and hcp-Li and then with bcc-Li, as well as preferred thermodynamic factors including the large dendrite formation energy and small migration barrier for Li. The prepared Li metal anode shows stable cycling in a wide current density range from 0.5 to 10.0 mA cm^–2. The LiFePO₄‖Li full cell fabricated with this Li metal anode exhibits only 9.5% capacity fading after 500 charge–discharge cycles at 1 C rate.