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As a technology for emerging environmental applications, water electrolysis is a significant approach for producing clean hydrogen energy. In this work, we used an efficacious piezoelectric method to significantly improve the catalytic water splitting activity without affecting the morphology as well as the components by altering the bulk charge separation state inside the material. The obtained CuCo2O4 nanorods were treated under a corona polarization apparatus, which significantly enhanced ferroelectricity relative to that before the polarization increasing the physical charge separation and piezoelectric potential energy, enhancing the green hydrogen production. The polarized CuCo2O4 nanorods exhibit excellent water electrolysis performance under alkaline conditions, with hydrogen evolution overpotential of 78.7 mV and oxygen evolution overpotential of 299 mV at 10 mA cm-2, which is much better than that of unpolarized CuCo2O4 nanorods. Moreover, the Tafel slopes of polarized CuCo2O4 nanorods are 86.9 mV dec-1 in the HER process and 73.1 mV dec-1 in the OER process, which are much lower than commercial catalysts of Pt/C (88.0 mV dec-1 for HER) or RuO2 (78.5 mV dec-1 for OER), proving faster kinetic on polarized CuCo2O4 nanorods due to their higher electroconductibility and intrinsic activity. In particular, polarized CuCo2O4 nanorods are identified as promising catalysts for water electrolysis with robust stability, offering outstanding catalytic performance and excellent energy efficiency.
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Poor cycling stability in lithium-sulfur (Li-S) batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures. Heterogeneous catalysis has emerged as a promising approach, leveraging the adsorption and catalytic performance on lithium polysulfides (LiPSs) to inhibit LiPSs shuttling and improve redox kinetics. In this study, we report an ultrathin and laminar SnO2@MXene heterostructure interlayer (SnO2@MX), where SnO2 quantum dots (QDs) are uniformly distributed across the MXene layer. The combined structure of SnO2 QDs and MXene, along with the creation of numerous active boundary sites with coordination electron environments, plays a critical role in manipulating the catalytic kinetics of sulfur species. The Li-S cell with the SnO2@MX-modified separator not only demonstrates superior electrochemical performance compared to cells with a bare separator but also induces homogeneous Li deposition during cycling. As a result, an areal capacity of 7.6 mAh cm-2 under a sulfur loading of 7.5 mg cm-2 and a high stability over 500 cycles are achieved. Our work demonstrates a feasible strategy of utilizing a laminar separator interlayer for advanced Li-S batteries awaiting commercialization and may shed light on the understanding of heterostructure catalysis with enhanced reaction kinetics.
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Quasi-solid polymer electrolyte (QPE) lithium (Li)-metal battery holds significant promise in the application of high-energy-density batteries, yet it suffers from low ionic conductivity and poor oxidation stability. Herein, a novel self-built electric field (SBEF) strategy is proposed to enhance Li+ transportation and accelerate the degradation dynamics of carbon-fluorine bond cleavage in LiTFSI by optimizing the termination of MXene. Among them, the SBEF induced by dielectric Nb4C3F2 MXene effectively constructs highly conductive LiF-enriched SEI and CEI stable interfaces, moreover, enhances the electrochemical performance of the QPE. The related Li-ion transfer mechanism and dual-reinforced stable interface are thoroughly investigated using ab initio molecular dynamics, COMSOL, XPS depth profiling, and ToF-SIMS. This comprehensive approach results in a high conductivity of 1.34â mS cm-1, leading to a small polarization of approximately 25â mV for Li//Li symmetric cell after 6000â h. Furthermore, it enables a prolonged cycle life at a high voltage of up to 4.6â V. Overall, this work not only broadens the application of MXene for QPE but also inspires the great potential of the self-built electric field in QPE-based high-voltage batteries.
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MXenes have aroused intensive enthusiasm because of their exotic properties and promising applications. However, to date, they are usually synthesized by etching technologies. Developing synthetic technologies provides more opportunities for innovation and may extend unexplored applications. Here, we report a bottom-up gas-phase synthesis of Cl-terminated MXene (Ti2CCl2). The gas-phase synthesis endows Ti2CCl2 with unique surface chemistry, high phase purity, and excellent metallic conductivity, which can be used to accelerate polysulfide conversion kinetics and dramatically prolong the cyclability of Li-S batteries. In-depth mechanistic analysis deciphers the origin of the formation of Ti2CCl2 and offers a paradigm for tuning MXene chemical vapor deposition. In brief, the gas-phase synthesis transforms the synthesis of MXenes and unlocks the hardly achieved potentials of MXenes.
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Separator engineering is a promising route to designing advanced lithium (Li) metal anodes for high-performance Li metal batteries (LMBs). Conventional separators are incapable of regulating the Li+ diffusion across the solid electrolyte interphase (SEI), leading to severe dendritic deposition. To address this issue, a polypropylene (PP) separator modified by spray coating the Cl-terminated titanium carbonitride MXene ink is designed (PP@Ti3CNCl2). The lithiophilic MXene provides excellent electrolyte wettability and low Li+ diffusion barriers, finally enhancing the Li+ diffusion kinetics of excessively stable SEI. The X-ray photoelectron spectroscopy depth profiling as well as cryo-transmission electron microscopy reveals that a gradient SEI hierarchy with evenly distributed LiF and LiCl is spontaneously formed during the electrochemical process. As a consequence, PP@Ti3CNCl2 delivers a high Coulombic efficiency (99.15%) coupled with a prolonged lifespan of over 5500 h in half cells and 3100 cycles at 2 C in full cells. This work offers an effective strategy for constructing dendrite-free and Li+ permeable interfaces toward high-energy-density LMBs.
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Design high-loading with superior activity and high atomic efficiency has consistently been a new frontier of heterogeneous catalysis while challenging in synthetic technology. In this work, a universal solid-state strategy is proposed for large scalable production of high-loading Ir clusters on porous hollow carbon nanobowls (Ir CSs/PHCNBs). The strong electronic interaction between metallic Ir cluster and C on PHCNBs leads to electron redistribution, which significantly improves the electron transfer rate on the interface. The obtained Ir CSs/PHCNBs only require overpotentials of 35, 34, and 37 mV for the hydrogen evolution reaction (HER) with stable outputting of 10 mA cm-2 under acidic, alkaline, and neutral conditions, respectively, which exceeds the state-of-the-art HER electrocatalysts. Meanwhile, the Tafel slopes of Ir CSs/PHCNBs for the HER process are 23.07, 48.76, and 28.95 mV dec-1 , greatly lower than that of PHCNBs (152.73, 227.96, and 140.29 mV dec-1 ) and commercial Pt/C (20%) (36.33, 66.10, and 36.61 mV dec-1 ). These results provide a new strategy for the universal synthesis of clusters catalysts and insight into understanding the interface effects between clusters and carbon substrate, facilitating the industrial application of hydrogen production.
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Two-dimensional (2D) transition metal carbides, and/or nitrides, so-called MXenes, have triggered intensive research interests in applications ranging from electrochemical energy storage to electronics devices. Producing these functional devices by printing necessitates to match the rheological properties of MXene dispersions to the requirements of various solution processing techniques. In particular, for additive manufacturing such as extrusion-printing, MXene inks with high solid fraction are typically required, which is commonly achieved by tediously removing excessive free water (top-down route). Here, the study reports on a bottom-up route to reach a highly concentrated binary MXene-water blend, so-called MXene dough, by controlling the water admixture to freeze-dried MXene flakes by exposure to water mist. The existence of a critical threshold of MXene solid content (≈60%), beyond which no dough is formed, or formed with compromised ductility is revealed. Such metallic MXene dough possesses high electrical conductivity, excellent oxidation stability, and can withstand a couple of months without apparent decay, providing that the MXene dough is properly stored at low-temperature with suppressed dehydration environment. Solution processing of the MXene dough into a micro-supercapacitor with gravimetric capacitance of 161.7 F g-1 is demonstrated. The impressive chemical and physical stability/redispersibility of MXene dough indicate its great promise in future commercialization.
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High energy density micro-supercapacitors (MSCs) are in high demand for miniaturized electronics and microsystems. Research efforts today focus on materials development, applied in the planar interdigitated, symmetric electrode architecture. A novel "cup & core" device architecture that allows for printing of asymmetric devices without the need of accurately positioning the second finger electrode here have been introduced. The bottom electrode is either produced by laser ablation of a blade-coated graphene layer or directly screen-printed with graphene inks to create grids with high aspect ratio walls forming an array of "micro-cups". A quasi-solid-state ionic liquid electrolyte is spray-deposited on the walls; the top electrode material -MXene inks- is then spray-coated to fill the cup structure. The architecture combines the advantages of interdigitated electrodes for facilitated ion-diffusion, which is critical for 2D-material-based energy storage systems by providing vertical interfaces with the layer-by-layer processing of the sandwich geometry. Compared to flat reference devices, volumetric capacitance of printed "micro-cups" MSC increased considerably, while the time constant decreased (by 58%). Importantly, the high energy density (3.99 µWh cm-2 ) of the "micro-cups" MSC is also superior to other reported MXene and graphene-based MSCs.
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Transparent conductive electrodes (TCEs) with a high figure of merit (FOMe, defined as the ratio of transmittance to sheet resistance) are crucial for transparent electronic devices, such as touch screens, micro-supercapacitors, and transparent antennas. Two-dimensional (2D) titanium carbide (Ti3C2Tx), known as MXene, possesses metallic conductivity and a hydrophilic surface, suggesting dispersion stability of MXenes in aqueous media allowing the fabrication of MXene-based TCEs by solution processing. However, achieving high FOMe MXene TCEs has been hindered mainly due to the low intrinsic conductivity caused by percolation problems. Here, we have managed to resolve these problems by (1) using large-sized Ti3C2Tx flakes (â¼12.2 µm) to reduce interflake resistance and (2) constructing compact microstructures by blade coating. Consequently, excellent optoelectronic properties have been achieved in the blade-coated Ti3C2Tx films, i.e., a DC conductivity of 19â¯325 S cm-1 at transmittances of 83.4% (≈6.7 nm) was obtained. We also demonstrate the applications of Ti3C2Tx TCEs in transparent Joule heaters and the field of supercapacitors, showing an outstanding Joule heating effect and high rate response, respectively, suggesting enormous potential applications in flexible, transparent electronic devices.
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Solution processing of two-dimensional nanomaterial inks guarantees efficient, straightforward fabrication of functional films, coatings, flexible devices, etc. Despite the excellent solution processibility and viscoelasticity of MXene aqueous inks, formulation of nonaqueous MXene inks with great affinity to both hydrophilic and hydrophobic substrates has proven quite challenging, limiting the practical applications of MXenes in printing/coatings on various substrates. Here, MXene surface chemistry is manipulated by asymmetrically grafting polystyrene and further concentrating the flakes into additive-free Janus MXene organic inks. The modified MXene nanosheets exhibit hydrophilicity on one side and hydrophobicity on the other. As a result, Janus MXene nanosheets ensure broad dispersibility in polar and nonpolar solvents, which in turn greatly extends the ink shelf life by slowing down the oxidation kinetics. Janus MXene sheets dispersed in toluene at room temperature remain at 90% of the initial solids after 1 month of storage. Janus surface engineering on MXene flakes guarantees the straightforward formation of uniform yet firm, large-area coatings on hydrophilic or hydrophobic substrates. These coatings demonstrate improved photothermal properties and chemical stability as well as good electromagnetic interference shielding performance. This strategy provides a simple and cost-effective way to promote the performance of MXene electronics in a variety of applications.
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Lithium sulfur (LiS) batteries possess high theoretical capacity and energy density, holding great promise for next generation electronics and electrical vehicles. However, the LiS batteries development is hindered by the shuttle effect and sluggish conversion kinetics of lithium polysulfides (LiPSs). Designing highly polar materials such as metal oxides (MOs) with moderate adsorption and effective catalytic activity is essential to overcome the above issues. To design efficient MOs catalysts, it is critical and necessary to understand the adsorption mechanism and associated catalytic processes of LiPSs. However, most reviews still lack a comprehensive investigation of the basic mechanism and always ignore their in-depth relationship. In this review, a systematic analysis toward understanding the underlying adsorption and catalytic mechanism in LiS chemistry as well as discussion of the typical works concerning MOs electrocatalysts are provided. Moreover, to improve the sluggish "adsorption-diffusion-conversion" process caused by the low conductive nature of MOs, oxygen vacancies and heterostructure engineering are elucidated as the two most effective strategies. The challenges and prospects of MOs electrocatalysts are also provided in the last section. The authors hope this review will provide instructive guidance to design effective catalyst materials and explore practical possibilities for the commercialization of LiS batteries.
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Background: Tuberculosis (TB) seriously threatens individual and public health. Recently, TB outbreaks in schools have been reported more frequently in China and have attracted widespread attention. We reported three TB outbreaks in high schools in Hunan Province, China. Methods: When a tuberculosis patient was reported in a school, we carried out field epidemiological investigations, including tuberculin skin testing (TST), chest X-ray (CXR) and laboratory test for all close contacts, and whole-genome sequencing (WGS) analyses to understand the transmission patterns, the causes and the risk factors for the outbreaks, thereby providing a foundation for the control of TB epidemics in schools. Results: A total of 49 students with TB patients were identified in the three schools where TB outbreaks occurred, including nine patients in School A, 14 patients in School B, and 26 patients in School C. In Schools A, B and C, the putative attack rates in the classes of the index case were 13.8% (8/58), 7.6% (5/66), and 40.4% (21/52), while the putative attack rates of expanding screening in the school were 0.3% (1/361), 0.2% (9/3955), and 0.2% (5/2080), respectively. Thirteen patients had patient delay, with a median delay interval of 69 days (IQR 30.5-113 days). Twelve patients had a healthcare diagnostic delay with a median delay interval of 32 days (IQR 24-82 days). Phylogenetic analysis of culture-positive patients revealed that most of them shared a small genetic distance (≤12 SNPs), with three separate genetic clusters (including one MDR-TB genomic cluster), indicating the recent transmission of Mycobacterium tuberculosis strains. Conclusion: This combination of field investigation and WGS analysis revealed the transmission of three TB outbreaks in schools. Reinforced implementation is needed to improve timely case finding and reduce diagnosis delay in routine TB control in the school population.
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Wireless technologies-supported printed flexible electronics are crucial for the Internet of Things (IoTs), human-machine interaction, wearable and biomedical applications. However, the challenges to existing printing approaches remain, such as low printing precision, difficulty in conformal printing, complex ink formulations and processes. Here we present a room-temperature direct printing strategy for flexible wireless electronics, where distinct high-performance functional modules (e.g., antennas, micro-supercapacitors, and sensors) can be fabricated with high resolution and further integrated on various flat/curved substrates. The additive-free titanium carbide (Ti3C2Tx) MXene aqueous inks are regulated with large single-layer ratio (>90%) and narrow flake size distribution, offering metallic conductivity (~6, 900 S cm-1) in the ultrafine-printed tracks (3 µm line gap and 0.43% spatial uniformity) without annealing. In particular, we build an all-MXene-printed integrated system capable of wireless communication, energy harvesting, and smart sensing. This work opens a door for high-precision additive manufacturing of printed wireless electronics at room temperature.
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Processing 2D materials into printable or coatable inks for the fabrication of functional devices has proven to be quite difficult. Additives are often used in large concentrations to address the processing challenges, but they drastically degrade the electronic properties of the materials. To remove the additives a high-temperature post-deposition treatment can be used, but this complicates the fabrication process and limits the choice of materials (i.e., no heat-sensitive materials). In this work, by exploiting the unique properties of 2D materials, a universal strategy for the formulation of additive-free inks is developed, in which the roles of the additives are taken over by van der Waals (vdW) interactions. In this new class of inks, which is termed "vdW inks", solvents are dispersed within the interconnected network of 2D materials, minimizing the dispersibility-related limitations on solvent selection. Furthermore, flow behavior of the inks and mechanical properties of the resultant films are mainly controlled by the interflake vdW attractions. The structure of the vdW inks, their rheological properties, and film-formation behavior are discussed in detail. Large-scale production and formulation of the vdW inks for major high-throughput printing and coating methods, as well as their application for room-temperature fabrication of functional films/devices are demonstrated.
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Objective@#To understand tuberculosis screening for newly enrolled students in Hunan Province and to provide reference for scholl based tuberculosis (TB) prevention and control.@*Methods@#During 2018 to 2020, TB screening was carried out for newly enrolled students in Hunan Province, and the screening results were statistically analyzed by descriptive analysis and χ 2 test.@*Results@#In 2018-2020, the average incidence rate of TB among students in Hunan Province was 20.90/100 000, with a decreasing trend by year ( χ 2 trend =89.45, P <0.01), the screening rate of TB in schools was 87.30%, and the screening rate for newly enrolled students was 86.81%, with downward trend by year ( χ 2 trend =2 843.34, 83 443.77, P <0.01). The proportion of suspicious symptoms, close contact, and active pulmonary TB patients among students were 0.53%, 0.21%, and 1.73/10 000, respectively, with decreasing trends by year( χ 2 trend =8 624.05, 2 215.48, 99.14, P <0.01). The proportion of strong positive PPD/ IGRA positive, changes in imaging examination and culturepositive of mycobacterium tuberculosis were 1.52%,0.20% and 12.40%, with increasing trends by year ( χ 2 trend =529.18, 147.65, 25.89, P <0.01). There were statistically significant differences in the proportion of suspicious symptoms, close contact, strong positive PPD/positive IGRA, changes in imaging examination and the proportion of patients with tuberculosis in the regional classification and school classification ( χ 2=529.18, 8 823.13, 705.63, 2 068.03, 1 299.00, 4 318.73 , 33.12, 2 329.07, 35.80, 1 781.65, P <0.01). There was no statistically significant difference in the proportion of culture positive of mycobacterium tuberculosis in the regional classification and school classification ( P >0.05).@*Conclusion@#The screening rate of newly enrolled student showed an upward trend, and the incidence rate of tuberculosis among students showed downward trend. Newly enrolled students among fresh students in high school have the highest PPD positive/IGRA positive rate and the proportion of pulmonary tuberculosis in the student population. It is necessary to increase the screening among fresh students in high school. In areas with conditions, tuberculosis screening of senior two students can be considered.
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Flexible transparent supercapacitors (FTSCs) are essential for the development of next-generation transparent electronics, however, a significant challenge is to achieve high-areal-capacitance FTSCs without sacrificing optical transparency. Herein, poly(3,4-ethylene dioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)-glued MoO3 nanowires anchored on the Ag nanofiber (AgNF) network are employed as FTSC film electrodes, in which the AgNF network provides primary conducting pathways and guarantees rapid electron transport, while wide-bandgap semiconductor MoO3 nanowires glued by the ultrathin PEDOT:PSS layer provide abundant redox-active sites to store energy. Benefiting from the PEDOT:PSS as the conducting glue to promote the connection at the junctions between AgNFs and MoO3 nanowires, the as-prepared AgNFs/MoO3/PEDOT:PSS (AMP) film electrode demonstrates a high transmittance (82.8%) and large areal capacitance (15.7 mF cm-2), and has outperformed all the transparent conductive films known to date. Even after 11 000 charge/discharge cycles, the capacitance still remains at 92.4% of the initial value. The assembled all-solid-state FTSC device delivers an energy density of 0.623 µW h cm-2, a power density of 40 µW cm-2, and excellent mechanical robustness, implying a great potential in high performance FTSCs.
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As a typical complex industrial process, hot rolling process (HRP) is different from chemical process. Strip steels are produced coil by coil, that means there is a long idle period between coils. The rolling speed is very high and the producing time of each coil is usually a few minutes. Previous researches mostly focus on fault detection in loaded condition and very few attempts have been made to exploit the monitoring of idle condition. In order to monitor the whole process, not only the loaded condition, but also the idle one, a novel nonlinear full condition process monitoring model is developed in this work. First, a dissimilarity index (DI) is defined for condition identification and a support data vector description (SVDD) model is established to monitor the idle condition. Second, t-distributed stochastic neighbor embedding (t-SNE) is used to extract nonlinear principal components (NPC) for slow feature analysis (SFA) and cointegration analysis (CA). Nonlinear cointegration analysis (NCA) can reveal the long-run dynamic relations of nonstationary parts, while nonlinear slow feature analysis (NSFA) can extract the latent temporal dynamic and static variations of stationary ones. Finally, the monitoring performance of the proposed model is verified through a real HRP.
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Designing lightweight nanostructured aerogels for high-performance electromagnetic interference (EMI) shielding is crucial yet challenging. Ultrathin cellulose nanofibrils (CNFs) are employed for assisting in building ultralow-density, robust, and highly flexible transition metal carbides and nitrides (MXenes) aerogels with oriented biomimetic cell walls. A significant influence of the angles between oriented cell walls and the incident EM wave electric field direction on the EMI shielding performance is revealed, providing an intriguing microstructure design strategy. MXene "bricks" bonded by CNF "mortars" of the nacre-like cell walls induce high mechanical strength, electrical conductivity, and interfacial polarization, yielding the resultant MXene/CNF aerogels an ultrahigh EMI shielding performance. The EMI shielding effectiveness (SE) of the aerogels reaches 74.6 or 35.5 dB at a density of merely 8.0 or 1.5 mg cm-3, respectively. The normalized surface specific SE is up to 189 400 dB cm2 g-1, significantly exceeding that of other EMI shielding materials reported so far.
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Alkali metals are ideal anodes for high-energy-density rechargeable batteries, while seriously hampered by limited cycle life and low areal capacities. To this end, rationally designed frameworks for dendrite-free and volume-changeless alkali-metal deposition at both high current densities and capacities are urgently required. Herein, a general 3D conductive Ti3C2TX MXene-melamine foam (MXene-MF) is demonstrated as an elastic scaffold for dendrite-free, high-areal-capacity alkali anodes (Li, Na, K). Owing to the lithiophilic nature of F-terminated MXene, conductive macroporous network, and excellent mechanical toughness, the constructed MXene-MF synchronously achieves a high current density of 50 mA cm-2 for Li plating, high areal capacity (50 mAh cm-2) with high Coulombic efficiency (99%), and long lifetime (3800 h), surpassing the Li anodes reported recently. Meanwhile, MXene-MF shows flat voltage profiles for 720 h at 10 mA cm-2 for the Na anode and 800 h at 5 mA cm-2 for the K anode, indicative of the wide applicability. Notably, the high current density of 20 mA cm-2 for 20 mAh cm-2 for the Na anode, accompanying good recyclability was rarely achieved before. When coupled with sulfur or Na3V2(PO4)3 cathodes, the assembled MXene-MF alkali (Li, Na)-based full batteries showcase enhanced rate capability and cycling stability, demonstrating the potential of MXene-MF for advanced alkali-metal batteries.
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MXenes are emerging rapidly as a new family of multifunctional nanomaterials with prospective applications rivaling that of graphenes. Herein, a timely account of the design and performance evaluation of MXene-based membranes is provided. First, the preparation and physicochemical characteristics of MXenes are outlined, with a focus on exfoliation, dispersion stability, and processability, which are crucial factors for membrane fabrication. Then, different formats of MXene-based membranes in the literature are introduced, comprising pristine or intercalated nanolaminates and polymer-based nanocomposites. Next, the major membrane processes so far pursued by MXenes are evaluated, covering gas separation, wastewater treatment, desalination, and organic solvent purification. The potential utility of MXenes in phase inversion and interfacial polymerization, as well as layer-by-layer assembly for the preparation of nanocomposite membranes, is also critically discussed. Looking forward, exploiting the high electrical conductivity and catalytic activity of certain MXenes is put into perspective for niche applications that are not easily achievable by other nanomaterials. Furthermore, the benefits of simulation/modeling approaches for designing MXene-based membranes are exemplified. Overall, critical insights are provided for materials science and membrane communities to navigate better while exploring the potential of MXenes for developing advanced separation membranes.