Energy Transfer Dynamics between Carbon Quantum Dots and Molybdenum Disulfide Revealed by Transient Absorption Spectroscopy

Zero-dimensional environmentally friendly carbon quantum dots(CQDs)combined with two-di-mensional materials have a wide range of applications in optoelec-tronic devices.We combined steady-state and transient absorp-tion spectroscopies to study the energy transfer dynamics between CQDs and molybdenum disulfide(MoS_(2)).Transient absorption plots showed photoinduced absorption and stimulated emission features,which involved the intrinsic and defect states of CQDs.Adding MoS_(2)to CQDs solution,the lowest unoccupied molecular orbital of CQDs transferred energy to MoS_(2),which quenched the intrinsic emission at 390 nm.With addition of MoS_(2),CQD-MoS_(2)composites quenched defect emission at 490 nm and upward absorption,which originated from another energy transfer from the defect state.Two energy transfer paths between CQDs and MoS_(2)were efficiently manipulated by changing the concentration of MoS_(2),which laid a foundation for improving device performance.

Properties of a MOS Device on Single Layer Molybdenum Disulfide

The properties of a metal-oxide-semiconductor device on a single layer MoS_(2)(molybdenum disulfide)semiconductor are determined theoretically utilizing the concept of physics that the carrier effective masses in materials are related to the intrinsic Fermi energy levels in materials by the universal mass-energy equivalence equation given as dE/E=dm/m,where E is the energy and m is the mass of the free electron.The known parameters of electron effective mass of 0.48 m and the direct bandgap of 1.8 eV for monolayer MoS_(2) semiconductor are utilized to determine the properties of the MOS(metal-oxide-semiconductor)device,with the given previous research consequence that the threshold for electron heating in SiO_(2) is 2 MV/cm-eV.

Hierarchical molybdenum disulfide nanosheet arrays stemmed from nickel-cobalt layered double hydroxide/carbon cloth for highly-efficient hydrogen evolution reaction

The hierarchical structure of molybdenum disulfide(MoS2)nanosheet arrays stemmed from nickelcobalt layered double hydroxide(NiCo-LDH)/carbon cloth was prepared by growing the MoS_(2) nanosheet arrays onto the NiCo-LDH template which was pre-deposited onto the carbon cloth substrate.In this electrode configuration,carbon cloth is the three dimensional and conductive skeleton;NiCo-LDH nanosheets,as the template,ensure the oriented growth of MoS2 nanosheet arrays.Therefore,more MoS_(2) active sites are exposed and the catalyst exhibits good hydrogen evolution reaction activity.

Developing polydopamine modified molybdenum disulfide/epoxy resin powder coatings with enhanced anticorrosion performance and wear resistance on magnesium lithium alloys

Epoxy resin powder coating has been successfully applied on the corrosion protection of magnesium lithium alloys.However,poor wear resistance and microcracks formed during the solidification have limited it extensive application.There are limited approaches to exploit such anti-corrosion and mechanical properties of magnesium lithium alloys.Herein,the epoxy resin powder coating with polydopamine modified molybdenum disulfide(MoS_(2)@PDA-EP powder coating with 0,0.1,0.2,0.5,1.0 wt.%loading)was well prepared by melt extrusion to investigate its anticorrosion performance and wear resistance.The results revealed that the addition of MoS_(2)@PDA enhanced the adhesion strength between coatings and alloys,wear resistance and corrosion protection of the powder coatings.Among them,the optimum was obtained by 0.2 wt.%MoS_(2)@PDA-EP powder coating which could be attributed to well dispersion and efficient adhesion with coating matrix.To conclude,MoS_(2)@PDA-EP powder coating is meaningfully beneficial for the anticorrosive and wear performance improvement of magnesium lithium alloys.

Molybdenum disulfide(MoS2)-based electrocatalysts for hydrogen evolution reaction:From mechanism to manipulation

Molybdenum disulfide(MoS_(2))-based materials as the non-noble metal catalysts have displayed the potential capability to drive electrocatalytic hydrogen evolution reaction(HER)for green hydrogen production along with their intrinsic activity,tunable electronic properties,low cost,and abundance reserves,which have attracted intensive attention as alternatives to the low-abundance and high-cost platinum-based catalysts.However,their insufficient catalytic HER activities and stability are the major challenges for them to become practically applicable.Hereby,the MoS_(2)-based electrocatalysts for HER are comprehensively reviewed to explain the fundamental science behind the manipulations of the crystal structure,microstructure,surface,and interface of MoS_(2) in order to enhance its catalytic performance through changing the electrical conductivity,the number of active sites,surface wettability,and the Gibbs free energy for hydrogen adsorption(ΔGH).Recent studies in surface/interface engineering,such as phase engineering,defect engineering,morphology design,and heterostructure construction,are analyzed to reveal the state-of-the-art strategies for designing and preparing the cost-effective and highperformance MoS_(2)-based catalysts through optimizing the charge transfer,surface-active sites,ΔGH,and surface hydrophilicity.Lastly,the perspectives,challenges,and future research directions of HER electrocatalysis are also given to facilitate the further research and development of HER catalysts.

Strong interactions in molybdenum disulfide heterostructures boosting the catalytic performance of water splitting: A short review

Two-dimensional materials(2DMs) have attracted substantial attention due to their abundant active sites and their ultrahigh surface area for different catalytic applications due to the high lateral-longitudinal ratio. Transition metal dichalcogenides(TMDs), especially MoS2, as one of the 2DMs most often studied, have shown superior activity in electrochemical applications. Recently, combinations of different 2DMs have been widely studied, and they appear to be the most promising strategy available to develop state of the art catalysts for different reactions.In this article, we review the interactions between MoS2 and other materials as well as the novel assembly induced phase transitions of TMDs and their underlying mechanisms. Several methods for inducing the phase transition of TMDs by building MoS2-based heterostructures have been introduced. The electronic coupling between these counterparts has significantly enhanced their conductivity and optimized the energy states of the materials, thus introducing enhanced activity as compared to their original counterparts. The ideas summarized in this article may shed new light on and help to develop next-generation green energy materials by designing and constructing highly active two-dimensional catalysts for efficient water splitting.

Tunable terahertz acoustic-phonon emission from monolayer molybdenum disulfide

The acoustic-phonon emission from monolayer molybdenum disulfide(ML-MoS_(2))driven by a direct-current electric field is studied theoretically using the Boltzmann equation method.It is found that the Cerenkov emission of terahertz acoustic-phonons can be generated when a very weak electric field is applied to ML-MoS_(2).The physical mechanisms of acoustic-phonon emission are analyzed from the perspective of condensed matter physics.The acoustic-phonon emission from ML-MoS_(2)is also compared with those from graphene and GaAs.The results reveal that the frequencies of acousticphonons generated by ML-MoS_(2)are between the frequencies of those generated from GaAs and graphene.The results of this work suggest that the ML-MoS_(2)can make up for graphene and GaAs in respect of acoustic-phonon emission and be used in tunable hypersonic devices such as terahertz sound sources.

Active MoS_(2)-based electrode for green ammonia synthesis

Nitrogen electro-reduction under mild conditions is one promising alternative approach of the energyconsuming Haber-Bosch process for the artificial ammonia synthesis.One critical aspect to unlocking this technology is to discover the catalysts with high selectivity and efficiency.In this work,the N_(2)-to-NH_(3)conversion on the functional MoS_(2)is fully investigated by density functional theory calculations since the layered MoS_(2)provides the ideal platform for the elaborating copies of the nitrogenase found in nature,wherein the functionalization is achieved via basal-adsorption,basal-substitution or edge-substitution of transition metal elements.Our results reveal that the edge-functionalization is a feasible strategy for the activity promotion;however,the basal-adsorption and basal-substitution separately suffer from the electrochemical instability and the NRR inefficiency.Specifically,MoS_(2)functionalized via edge W-substitution exhibits an exceptional activity.The energetically favored reaction pathway is through the distal pathway and a limiting potential is less than 0.20 V.Overall,this work escalates the rational design of the high-effective catalysts for nitrogen fixation and provides the explanation why the predicated catalyst have a good performance,paving the guidance for the experiments.

High-throughput calculation-based rational design of Fe-doped MoS_(2) nanosheets for electrocatalytic p H-universal overall water splitting

Electrocatalytic water splitting is crucial for H2generation via hydrogen evolution reaction(HER)but subject to the sluggish dynamics of oxygen evolution reaction(OER).In this work,single Fe atomdoped MoS_(2)nanosheets(SFe-DMNs)were prepared based on the high-throughput density functional theory(DFT)calculation screening.Due to the synergistic effect between Fe atom and MoS_(2)and optimized intermediate binding energy,the SFe-DMNs could deliver outstanding activity for both HER and OER.When assembled into a two-electrode electrolytic cell,the SFe-DMNs could achieve the current density of 50 mA cm^(-2)at a low cell voltage of 1.55 V under neutral condition.These results not only confirmed the effectiveness of high-throughput screening,but also revealed the excellent activity and thus the potential applications in fuel cells of SFe-DMNs.

Emerging MoS_(2)Wafer-Scale Technique for Integrated Circuits

As an outstanding representative of layered materials,molybdenum disulfide(MoS_(2))has excellent physical properties,such as high carrier mobility,stability,and abundance on earth.Moreover,its reasonable band gap and microelectronic compatible fabrication characteristics makes it the most promising candidate in future advanced integrated circuits such as logical electronics,flexible electronics,and focal-plane photodetector.However,to realize the all-aspects application of MoS_(2),the research on obtaining high-quality and large-area films need to be continuously explored to promote its industrialization.Although the MoS_(2)grain size has already improved from several micrometers to sub-millimeters,the high-quality growth of wafer-scale MoS_(2)is still of great challenge.Herein,this review mainly focuses on the evolution of MoS_(2)by including chemical vapor deposition,metal–organic chemical vapor deposition,physical vapor deposition,and thermal conversion technology methods.The state-of-the-art research on the growth and optimization mechanism,including nucleation,orientation,grain,and defect engineering,is systematically summarized.Then,this review summarizes the wafer-scale application of MoS_(2)in a transistor,inverter,electronics,and photodetectors.Finally,the current challenges and future perspectives are outlined for the wafer-scale growth and application of MoS_(2).

Pea-like MoS_(2)@NiS_(1.03)-carbon heterostructured hollow nanofibers for high-performance sodium storage

The rational synergy of chemical composition and spatial nanostructures of electrode materials play important roles in high-performance energy storage devices.Here,we designed pea-like MoS_(2)@NiS_(1.03)-carbon hollow nanofibers using a simple electrospinning and thermal treatment method.The hierarchical hollow nanofiber is composed of a nitrogen-doped carbon-coated NiS_(1.03) tube wall,in which pea-like uniformly discrete MoS_(2) nanoparticles are enclosed.As a sodium-ion battery electrode material,the MoS_(2)@NiS_(1.03)-carbon hollow nanofibers have abundant diphasic heterointerfaces,a conductive network,and appropriate volume variation-buffering spaces,which can facilitate ion diffusion kinetics,shorten the diffusion path of electrons/ion,and buffer volume expansion during Na^(+)insertion/extraction.It shows outstanding rate capacity and long-cycle performance in a sodium-ion battery.This heterogeneous hollow nanoarchitectures designing enlightens an efficacious strategy to boost the capacity and long-life stability of sodium storage performance of electrode materials.

Covalent-architected molybdenum disulfide arrays on Ti_(3)C_(2)T_(x) MXene fiber towards robust capacitive energy storage

Ti_(3)C_(2)T_(x)MXene fiber has shown extraordinary potential for supercapacitor electrode in wearable elec-tronics and textile energy storage,but realizing high energy density and practical-powered applications remains a great challenge.Here,we report a covalent-architected molybdenum disulfide-Ti_(3)C_(2)T_(x)(MoS_(2)-Ti_(3)C_(2)T_(x))core-shell fiber for high-performance supercapacitor.Benefiting from the microfluidic and micro-reaction strategies,the ordered MoS_(2)arrays are strongly bridged on Ti_(3)C_(2)T_(x)fiber via Ti-O-Mo bond,re-sulting in large exposed surface,enhanced porosity and excellent interfacial conduction for charges high diffusion and faradaic transfer.The MoS_(2)-Ti_(3)C_(2)T_(x)fiber exhibits ultra-large capacitance of 2028 F cm^(-3)and admirable reversibility in 1 M H_(2)SO_(4)aqueous electrolyte.Meanwhile,MoS_(2)-Ti_(3)C_(2)T_(x)fiber-based solid-state supercapacitor presents high energy density of 23.86 mWh cm^(-3),capacitance of 1073.6 F cm^(-3)and superior cycling ability of 92.13%retention after 20,000 cycles,which can realize stable energy supply for wearable watch,LEDs,electric fans,toy ship and self-powered devices.Our work may provide an insight-ful guidance for the advanced design of structural fiber towards robust new energy and next-generation wearable industry.

Oriented molybdenum disulfide-silica/hydrogenated nitrile butadiene rubber composites:Effects of nanosheets on mechanical and dielectric properties

A series of non-covalently functionalized molybdenum disulfide-silica(f-MoS_(2)-SiO_(2))nanocomposites was prepared by an in-situ assembled method and used to fabricate the oriented molybdenum disulfide-SiO_(2)/Hydrogenated Nitrile Butadiene Rubber(f-MoS2-SiO_(2)/HNBR)composites.The characterization results show the synergistic dispersion between the functionalized molybdenum disulfide(f-MoS2)nanosheets and SiO_(2)nanoparticles.The addition of f-MoS2 nanosheets can improve the dispersion of fillers in the rubber matrix and weaken the filler network.The non-covalently functionalization improves the interface interaction between f-MoS_(2)nanosheets and the rubber matrix.Furthermore,the tensile strength of f-MoS2-SiO_(2)/HNBR is 65.9%higher than that of SiO_(2)/HNBR by adding 1.0wt%of f-MoS_(2).At the same time,the dielectric constant of f-MoS2-SiO_(2)/HNBR is increased by 23.7%compared to SiO_(2)/HNBR due to the micro-capacitor structure of parallel f-MoS2 nanosheets in the rubber matrix.Our work provides new ideas for the development of high-performance elastomer materials.

Molybdenum disulfide@nickel phyllosilicate hybrid for improving the flame retardancy and wear resistance of epoxy composites

In this study,nickel phyllosilicate was synthesized based on molybdenum disulfide(MoS2@NiPS)by the sol-gel method,and then MoS2@NiPS was used to prepare epoxy composites.The thermal stability,flame retardancy,and frictional performances of epoxy composites were studied.With the addition of 3 wt%MoS2@NiPS,the epoxy composite increased the limiting oxygen index from 23.8%to 26.1%and reduced the vertical burning time from 166 s for epoxy resin to 35 s.The residual char of the epoxy composite increased from 11.8 to 20.2 wt%.MoS2@NiPS promoted the graphitization of the residual char,and facilitated the formation of a dense and continuous char layer,thereby improving the fire safety of epoxy resin.The epoxy composite with 3 wt%MoS2@NiPS had excellent wear resistance property with a wear rate of 2.19×10^(‒5) mm^(3)·N^(-1)·m^(-1),which was 68.8%lower than that of epoxy resin.This study presented a practical approach to improve the frictional and fire resistance of epoxy composites.

Ordered Macroporous MoS_(2)-Carbon Composite with Fast and Robust Sodium Storage Properties to Solve the Issue of Kinetics Mismatch of Sodium-Ion Capacitors

Metal-ion capacitors(including Li^(+),Na^(+),and K^(+))effectively combine a battery negative electrode capable of reversibly intercalating metal cations,together with an electrical double-layer positive electrode.However,such novel cell design has a birth defect,namely kinetics mismatch between sluggish negative electrode and fast positive electrode,thus limiting the energy-power performance.Herein,we design a MoS_(2)-carbon composite anode with the ordered macroporous architecture and interlayer-expanded feature,exhibiting the fast and reversible Na^(+)redox processes.This kinetically favored anode is coupled with a homemade activated carbon cathode that allows for the excellent electrochemical performance of sodiumion capacitor with respect to large specific capacity,high-rate capability,and robust cycling.Through quantification of the potential swings of anode and cathode via a three-electrode Swagelok cell,we for the first time observe the abnormal variation law of potential swings and thus directly providing the evidence that the kinetics gap has been filled up by this kinetically favored anode.Our results represent a crucial step toward understanding the key issues of kinetics mismatch for hybrid cell,thus propelling the development of design of kinetically favored anode materials for high-performance metalion capacitors.

Mechanism of catalytic hydropyrolysis of sedimentary organic matter with MoS_2

MoS2 was used as an efficient catalyst for hydropyrolysis （Hypy） of three samples of sedimentary organic matter with different maturities. Through comparison with Soxhlet extraction （SE）, it was found that MoS2 catalytic Hypy can remarkably promote the yields of total chloroform extracts, saturates, aromatics, hopanes and steranes. In addition, the difference of biomarker parameters indicated that isomerization of covalently-bound biomarkers is much more difficult than their free counterparts. Meanwhile, the high conversion of total organic carbon （TOC） in MoS2 catalytic Hypy of organic matter proved that the presence of dispersed molybdenum sulfide accelerated the breaking of C-C bonds and the release of hydrocarbons. To address the catalytic mechanism, a series of control experiments based on free Hypy and catalytic Hypy were conducted. The results showed that the calculated atomic ratio of carbon conversion/hydrogen conversion for catalytic Hypy was much larger than the presumed value of 1/2, indicating that intensive hydrogenation took place and significantly influenced the distribution of liquid products. Analysis of stable hydrogen isotope data, infrared spectra and m/z 83 ion chromatograph of the saturate fraction further confirmed this hypothesis. The difference of S content changing （AS） between catalyst-free Hypy and catalytic Hypy, and the thermal characteristics of the catalyst, indicated that active H2S was definitely generated and it probably initiated free radical reactions in the early stage of hydropyrolysis of organic matter.

Boosting pH-Universal Hydrogen Evolution of Molybdenum Disulfide Particles by Interfacial Engineering

The design of high-efficiency non-noble and earth-abundant electrocatalysts for hydrogen evolution reaction(HER)is highly paramount for water splitting and renewable energy systems.Molybdenum disulfide(MoS_(2))with abundant edge sites can be utilized as a promising alternative,but its catalytic activity is greatly related to the pH values,especially in an alkaline environment due to the extremely high energy barriers for water adsorption and dissociation steps.Here we report an exceptionally efficient and stable electrocatalyst to improve the sluggish HER process of layered MoS_(2)particles in different pH electrolytes,especially in base.The electrocatalyst is constructed by in situ growing selenium-doped MoS_(2)(Se-MoS_(2))nanoparticles on three-dimensional cobalt nickel diselenide(mCo_(0.2)Ni_(0.8)Se_(2))nanostructured arrays.Due to the large number of active edge sites of Se-MoS_(2)particles exposed at the surface,robust electrical conductivity and large surface area of mCo_(0.2)Ni_(0.8)Se_(2)support,and strong interfacial interactions between Se-MoS_(2)and mCo_(0.2)Ni_(0.8)Se_(2),this hybrid catalyst shows very outstanding catalytic HER properties featured by low overpotentials of 30 and 122 mV at 10 and 100 mA/cm^(2)with good operational stability in base,respectively,which outperforms most of inexpensive catalysts consisting of layered MoS_(2),transition metal selenides and sulfides,and it performs as well as noble Pt catalysts.Meanwhile,this electrocatalyst is also very active in neutral and acidic electrolytes,requiring low overpotentials of 93 and 94 mV at 10 mA/cm^(2),respectively,demonstrating its superb pH universality as a HER electrocatalyst with excellent catalytic durability.This study provides a straightforward strategy to construct an efficient non-noble electrocatalyst for driving the HER kinetics in different electrolytes.

Consistency-dependent optical properties of lubricating grease studied by terahertz spectroscopy

The optical properties of four kinds of lubricating greases （urea, lithium, extreme pressure lithium, molybdenum disulfide lithium greases） with different NLGL （National Lubricant Grease Institute of America） numbers were investigated using terahertz time-domain spectroscopy. Greases with different NLGL grades have unique spectral features in the terahertz range. Comparison of the experimental data with predictions based on Lorentz Lorenz theory exhibited that the refractive indices of each kind of lubricating grease were dependent on the their consistency. In addition, molybdenum disullfide （MoS2） aa a libricant additive shows strong absorption from 0.2 to 1.4 THz, leading to higher absorption of MoS2-1ithium grease than that of lithium grease.

Highly sensitive piezoresistive pressure sensors based on laser-induced graphene with molybdenum disulfide nanoparticles

Wearable pressure sensors have drawn significant attention because of their extensive applications in motion detection, tactile sensing, and health monitoring. However, the complex manufacturing process and high cost of active materials make low-cost,large-scale production elusive. In this work, we report a flexible piezoresistive pressure sensor assembled with two 3D laserinduced graphene(LIG) foam electrodes on a polyimide thin film from a simple laser scribing process in the ambient environment. The design of the air gap between the two foam electrodes allows the sensor to showcase a low limit of detection of 0.274 Pa, which provides favorable sensing performance in motion detection and wrist pulse monitoring. The addition of spherical MoS2 nanoparticles between the two foam electrodes further enhances the sensitivity to 88 k Pa-1 and increases the sensing range to significantly outperform the previous literature reports. The demonstrated LIG pressure sensors also exhibit fast response/recovery rates and excellent durability/repeatability.

Revisiting lithium-storage mechanisms of molybdenum disulfide

Molybdenum disulfide(MoS_(2)),a typical two-dimensional transition metallic layered material,attracts tremendous attentions in the electrochemical energy storage due to its excellent physicochemical properties.However,with the deepening of the research and exploration of the lithium storage mechanism of these advanced MoS_(2)-based anode materials,the complex reaction process influenced by internal and external factors hinders the exhaustive understanding of the lithium storage process.To design stable anode material with high performance,it is urgent to review the mechanisms of reported anode materials and summarize the related factors that influence the reaction processes.This review aims to dissect all possible side reactions during charging and discharging process,uncover internal and external factors inducing various anode reactions and finally put forward strategies of controlling high cycling capacity and super-stable lithium storage capability of MoS_(2).This review will be helpful to the design of MoS_(2)-based lithium-ion batteries(LIBs) with excellent cycle performance to enlarge the application fields of these advanced electrochemical energy storage devices.