Synthesis of Ti_2CT_x MXene as electrode materials for symmetric supercapacitor with capable volumetric capacitance

Two-dimensional(2D)metal carbides,MXene,present the promising application for the energy storage system.Among the MXene family,Ti_2CT_xas the lightest material,shows its unique electrochemical performance.Herein,Ti_2CT_xis synthesized by selective etching Al layer from the Ti_2Al C.With the optimized HF treating condition,Ti_2CT_xdisplays high volumetric capacitance and remarkable rate ability.Moreover,the Ti_2CT_x//Ti_2CT_xsymmetric supercapacitor is designed and assembled,which presents capable capacitance,outstanding rate performance and excellent cycling performance.The remarkable electrochemical performance is attributed to its 2D structure and high electronic conductivity.This work demonstrates the potential application of the Ti_2CT_xfor the supercapacitors and provides a template to design highperformance supercapacitors with 2D electrode materials.

Evaluation of performance of machine learning methods in mining structure-property data of halide perovskite materials

With the rapid development of artificial intelligence and machine learning(ML)methods,materials science is rapidly entering the era of data-driven materials informatics.ML models serve as the most crucial component,closely bridging material structure and material properties.There is a considerable difference in the prediction performance of different ML methods for material systems.Herein,we evaluated three categories(linear,kernel,and nonlinear methods)of models,with twelve ML algorithms commonly used in the materials field.In addition,halide perovskite was chosen as an example to evaluate the fitting performance of different models.We constructed a total dataset of 540 halide perovskites and 72 features,with formation energy and bandgap as target properties.We found that different categories of ML models show similar trends for different target properties.Among them,the difference between the models is enormous for the formation energy,with the coefficient of determination(R2)range 0.69-0.953.The fitting performance between the models is closer for bandgap,with the R^(2)range 0.941-0.997.The nonlinear-ensemble model shows the best fitting performance for both the formation energy and the bandgap.It shows that the nonlinear-ensemble model,constructed by combining multiple weak learners,effectively describes the nonlinear relationship between material features and target property.In addition,the extreme gradient boosting decision tree model shows the most superior results among all the models and searches for two new descriptors that are crucial for formation energy and bandgap.Our work provides useful guidance for the selection of effective machine learning methods in the data-mining studies of specific material systems.

Advances in the Application of Perovskite Materials

Nowadays, the soar of photovoltaic performance of perovskite solar cells has set off a fever in the study of metal halide perovskite materials. The excellent optoelectronic properties and defect tolerance feature allow metal halide perovskite to be employed in a wide variety of applications. This article provides a holistic review over the current progress and future prospects of metal halide perovskite materials in representative promising applications, including traditional optoelectronic devices(solar cells, light-emitting diodes, photodetectors, lasers), and cutting-edge technologies in terms of neuromorphic devices(artificial synapses and memristors) and pressure-induced emission. This review highlights the fundamentals, the current progress and the remaining challenges for each application, aiming to provide a comprehensive overview of the development status and a navigation of future research for metal halide perovskite materials and devices.

High pressure structural phase transitions of TiO_2 nanomaterials

Recently, the high pressure study on the TiO_2 nanomaterials has attracted considerable attention due to the typical crystal structure and the fascinating properties of TiO_2 with nanoscale sizes. In this paper, we briefly review the recent progress in the high pressure phase transitions of TiO_2 nanomaterials. We discuss the size effects and morphology effects on the high pressure phase transitions of TiO_2 nanomaterials with different particle sizes, morphologies, and microstructures. Several typical pressure-induced structural phase transitions in TiO_2 nanomaterials are presented, including size-dependent phase transition selectivity in nanoparticles, morphology-tuned phase transition in nanowires, nanosheets,and nanoporous materials, and pressure-induced amorphization（PIA） and polyamorphism in ultrafine nanoparticles and TiO_2-B nanoribbons. Various TiO_2 nanostructural materials with high pressure structures are prepared successfully by high pressure treatment of the corresponding crystal nanomaterials, such as amorphous TiO_2 nanoribbons, α-PbO_2-type TiO_2 nanowires, nanosheets, and nanoporous materials. These studies suggest that the high pressure phase transitions of TiO_2 nanomaterials depend on the nanosize, morphology, interface energy, and microstructure. The diversity of high pressure behaviors of TiO_2 nanomaterials provides a new insight into the properties of nanomaterials, and paves a way for preparing new nanomaterials with novel high pressure structures and properties for various applications.

High-Pressure Preparation of High-Density Cu_2ZnSnS_4 Materials

High-density Cu2ZnSnS4 （CZTS） materials are prepared via the mechanical alloying and high pressure sintering method using Cu2S, ZnS and SnS2 as the raw materials. The morphological, structural, compositional and electrical properties of the materials are investigated by using x-ray diffraction, scanning electron microscopy, and energy dispersive x-ray spectroscopy, as well as by the Raman scattering and the Hall EFfect measurements. The CZTS synthesized under 5 GPa and 800℃ shows a p-type conductivity, with a resistivity of 9.69 × 10^-2 Ω.cm and a carrier concentration of 1.45 × 10^20 cm-3. It is contributed to by the large grains in the materials reducing the grain boundaries, thus effectively reducing the recombination of the charge carriers.

Investigating the thermal conductivity of materials by analyzing the temperature distribution in diamond anvils cell under high pressure

Investigating the thermal transport properties of materials is of great importance in the field of earth science and for the development of materials under extremely high temperatures and pressures.However,it is an enormous challenge to characterize the thermal and physical properties of materials using the diamond anvil cell(DAC)platform.In the present study,a steady-state method is used with a DAC and a combination of thermocouple temperature measurement and numerical analysis is performed to calculate the thermal conductivity of the material.To this end,temperature distributions in the DAC under high pressure are analyzed.We propose a three-dimensional radiative-conductive coupled heat transfer model to simulate the temperature field in the main components of the DAC and calculate in situ thermal conductivity under high-temperature and high-pressure conditions.The proposed model is based on the finite volume method.The obtained results show that heat radiation has a great impact on the temperature field of the DAC,so that ignoring the radiation effect leads to large errors in calculating the heat transport properties of materials.Furthermore,the feasibility of studying the thermal conductivity of different materials is discussed through a numerical model combined with locally measured temperature in the DAC.This article is expected to become a reference for accurate measurement of in situ thermal conductivity in DACs at high-temperature and high-pressure conditions.

Sequestration of helium and xenon via iron-halide compounds in early Earth

The terrestrial abundance anomalies of helium and xenon suggest the presence of deep-Earth reservoirs of these elements,which has led to great interest in searching for materials that can host these usually unreactive elements.Here,using an advanced crystal structure search approach in conjunction with first-principles calculations,we show that several Xe/He-bearing iron halides are thermodynamically stable in a broad region of P–T phase space below 60 GPa.Our results present a compelling case for sequestration of He and Xe in the early Earth and may suggest their much wider distribution in the present Earth than previously believed.These findings offer insights into key material-based and physical mechanisms for elucidating major geological phenomena.

Scanning the energy dissipation process of energetic materials based on excited state relaxation and vibration–vibration coupling

The energy dissipation mechanism of energetic materials（EMs） is very important for keeping safety. We choose nitrobenzene as a model of EM and employ transient absorption（TA） spectroscopy and time-resolved coherent anti-stokes Raman scattering（CARS） to clarify its energy dissipation mechanism. The TA data confirms that the excited nitrobenzene spends about 16 ps finishing the twist intramolecular charge transfer from benzene to nitro group, and dissipates its energy through the rapid vibration relaxation in the initial excited state. And then the dynamics of vibrational modes（VMs） in the ground state of nitrobenzene, which are located at 682 cm^-1（v1）, 854 cm^-1（v2）, 1006 cm^-1（v3）, and 1023 cm^-1（v4）,is scanned by CARS. It exhibits that the excess energy of nitrobenzene on the ground state would further dissipate through intramolecular vibrational redistribution based on the vibrational cooling of vi and v2 modes, v1 and v4 modes, and v3 and v4 modes. Moreover, the vibration-vibration coupling depends not only on the energy levels of VMs, but also on the spatial position of chemical bonds relative to the VM.

Theoretical design of diamondlike superhard structures at high pressure

Diamond, as the hardest known material, has been widely used in industrial applications as abrasives, coatings, and cutting and polishing tools, but it is restricted by several shortcomings, e.g., its low thermal and chemical stability. Considerable efforts have been devoted to designing or synthesizing the diamond-like B-C-N-O compounds, which exhibit excellent mechanical property. In this paper, we review the recent theoretical design of diamond-like superhard structures at high pressure. In particular, the recently designed high symmetric phase of low-energy cubic BC3 meets the experimental observation, and clarifies the actual existence of cubic symmetric phase for the compounds formed by B-C-N-O system,besides the classical example of cubic boron nitride.

Role of self-assembled molecules’anchoring groups for surface defect passivation and dipole modulation in inverted perovskite solar cells

Inverted perovskite solar cells have gained prominence in industrial advancement due to their easy fabrication,low hysteresis effects,and high stability.Despite these advantages,their efficiency is currently limited by excessive defects and poor carrier transport at the perovskite-electrode interface,particularly at the buried interface between the perovskite and transparent conductive oxide(TCO).Recent efforts in the perovskite community have focused on designing novel self-assembled molecules(SAMs)to improve the quality of the buried interface.However,a notable gap remains in understanding the regulation of atomic-scale interfacial properties of SAMs between the perovskite and TCO interfaces.This understanding is crucial,particularly in terms of identifying chemically active anchoring groups.In this study,we used the star SAM([2-(9H-carbazol-9-yl)ethyl]phosphonic acid)as the base structure to investigate the defect passivation effects of eight common anchoring groups at the perovskite-TCO interface.Our findings indicate that the phosphonic and boric acid groups exhibit notable advantages.These groups fulfill three key criteria:they provide the greatest potential for defect passivation,exhibit stable adsorption with defects,and exert significant regulatory effects on interface dipoles.Ionized anchoring groups exhibit enhanced passivation capabilities for defect energy levels due to their superior Lewis base properties,which effectively neutralize local charges near defects.Among various defect types,iodine vacancies are the easiest to passivate,whereas iodine-substituted lead defects are the most challenging to passivate.Our study provides comprehensive theoretical insights and inspiration for the design of anchoring groups in SAMs,contributing to the ongoing development of more efficient inverted perovskite solar cells.

Systematical High-Pressure Study of Praseodymium Nitrides in N-Rich Region

We investigate high-pressure phase diagrams of Pr–N compounds by proposing five stable structures(PnmaPr N,Ⅰ4/mmm-PrN_(2),C2/m-PrN_(3),P■-PrN_(4),and R3-PrN_(8))and two metastable structures(P■-PrN_(6)and P■-PrN_(10)).The P■-PrN_(6)with the N14-ring layer and R3-PrN_(8)with the N18-ring layer can be quenched to ambient conditions.For the P■-PrN_(10),the N_(22)-ring layer structure transfers into infinite chains with the pressure quenched to ambient pressure.Remarkably,a novel polynitrogen h R8-N designed by the excision of Pr atoms from R3-PrN_(8)is obtained and can be quenched to ambient conditions.The N-rich structures of P■-PrN_(6),R3-PrN_(8),c-PrN_(10)and the solid pure nitrogen structure exhibit outstanding properties of energy density and explosive performance.

Interception of Layered LP-N and HLP-N at Ambient Conditions by Confined Template

We propose a feasible strategy of intercepting the layered polymeric nitrogen(LP-N)and hexagonal layered polymeric nitrogen(HLP-N)at ambient conditions by using the confinement templates.The stable mechanism of confined LP-N and HLP-N at ambient conditions is revealed.

Influence of Local Cation Order on Electronic Structure and Optical Properties of Cation-Disordered Semiconductor AgBiS_(2)

Site disorder exists in some practical semiconductors and can significantly impact their intrinsic properties both beneficially and detrimentally.However,the uncertain local order and structure pose a challenge for experimental and theoretical research.Especially,it hinders the investigation of the effects of the diverse local atomic environments resulting from the site disorder.We employ the special quasi-random structure method to perform first-principles research on connection between local site disorder and electronic/optical properties,using cationdisordered AgBiS_(2)(rock salt phase)as an example.We predict that cation-disordered AgBiS_(2)has a bandgap ranging from 0.6 to 0.8 eV without spin-orbit coupling and that spin-orbit coupling reduces this by approximately 0.3 eV.We observe the effects of local structural features in the disordered lattice,such as the one-dimensional chain-like aggregation of cations that results in formation of doping energy bands near the band edges,formation and broadening of band-tail states,and the disturbance in the local electrostatic potential,which significantly reduces the bandgap and stability.The influence of these ordered features on the optical properties is confined to alterations in the bandgap and does not markedly affect the joint density of states or optical absorption.Our study provides a research roadmap for exploring the electronic structure of site-disordered semiconductor materials,suggests that the ordered chain-like aggregation of cations is an effective way to regulate the bandgap of AgBiS_(2),and provides insight into how variations in local order associated with processing can affect properties.

Tailoring bimodal grain structure of Mg-9Al-1Zn alloy for strength-ductility synergy:Co-regulating effect from coarse Al_(2)Y and submicron Mg_(17)Al_(12) particles

Grain boundary strengthening is an effective strategy for increasing mechanical properties of Mg alloys.However,this method offers limited strengthening in bimodal grain-structured Mg alloys due to the difficultly in increasing the volume fraction of fine grains while keeping a small grain size.Herein,we show that the volume fraction of fine grains(FGs,~2.5μm)in the bimodal grain structure can be tailored from~30 vol.%in Mg-9 Al-1 Zn(AZ91)to~52 vol.%in AZ91-1Y(wt.%)processed by hard plate rolling(HPR).Moreover,a superior combination of a high ultimate tensile strength(~405 MPa)and decent uniform elongation(~9%)is achieved in present AZ91-1Y alloy.It reveals that a desired bimodal grain structure can be tailored by the co-regulating effect from coarse Al_(2)Y particles resulting in inhomogeneous recrystallization,and dispersed submicron Mg_(17)Al_(12)particles depressing the growth of recrystallized grains.The findings offer a valuable insight in tailoring bimodal grain-structured Mg alloys for optimized strength and ductility.

Inclusions in large diamond single crystals at different temperatures of synthesis

The inclusions in large diamond single crystals have effects on its ultimate performance, which restricts its industrial applications to a great extent. Therefore, it is necessary to study the inclusions systematically. In this paper, large diamond single crystals with different content values of inclusions are synthesized along the(100) surface by the temperature gradient method(TGM) under 5.6 GPa at different temperatures. With the synthetic temperature changing from 1200?C to 1270?C,the shapes of diamonds change from plate to low tower, to high tower, even to steeple. From the microscopic photographs of the diamond samples, it can be observed that with the shapes of the samples changing at different temperatures, the content values of inclusions in diamonds become zero, a little, much and most, correspondingly. Consequently, with the temperature growing from low to high, the content values of inclusions in crystals increase. The origin of inclusions is explained by the difference in growth rate between diamond crystal and its surface. The content values of inclusions in diamond samples are quantitatively calculated by testing the densities of diamond samples. And the composition and inclusion content are analyzed by energy dispersive spectroscopy(EDS) and x-ray diffraction(XRD). From contrasting scanning electron microscopy(SEM) photographs, it can be found that the more the inclusions in diamond, the more imperfect the diamond surface is.

Growth and annealing study of hydrogen-doped single diamond crystals under high pressure and high temperature

A series of diamond crystals doped with hydrogen is successfully synthesized using LiH as the hydrogen source in a catalyst-carbon system at a pressure of 6.0 GPa and temperature ranging from 1255 C to 1350 C.It is shown that the high temperature plays a key role in the incorporation of hydrogen atoms during diamond crystallization.Fourier transform infrared micro-spectroscopy reveals that most of the hydrogen atoms in the synthesized diamond are incorporated into the crystal structure as sp 3-CH 2-symmetric（2850 cm-1） and sp 3 CH 2-antisymmetric vibrations（2920 cm-1）.The intensities of these peaks increase gradually with an increase in the content of the hydrogen source in the catalyst.The incorporation of hydrogen impurity leads to a significant shift towards higher frequencies of the Raman peak from 1332.06 cm-1 to 1333.05 cm-1 and gives rise to some compressive stress in the diamond crystal lattice.Furthermore,hydrogen to carbon bonds are evident in the annealed diamond,indicating that the bonds that remain throughout the annealing process and the vibration frequencies centred at 2850 and 2920 cm-1 have no observable shift.Therefore,we suggest that the sp 3 C-H bond is rather stable in diamond crystals.

Fabrication and characteristics of nitrogen-doped nanocrystalline diamond/p-type silicon heterojunction

Nitrogen-doped nanocrystalline diamond films(N-NDFs)have been deposited on p-type silicon(Si)by microwave plasma chemical vapor deposition.The reaction gases are methane,hydrogen,and nitrogen without the conventional argon(Ar).The N-NDFs were characterized by X-ray diffraction,Raman spectroscopy,and scanning electron microscopy.The grain sizes are of 8~10 nm in dimension.The N-NDF shows n-type behavior and the corresponding N-NDF/p-Si heterojunction diodes are realized with a high rectification ratio of 102 at^7.8 V,and the current density reaches to1.35 A/cm2 at forward voltage of 8.5 V.The findings suggest that fabricated by CH_4/H_2/N_2 without Ar,the N-NDFs and the related rectifying diodes are favorable for achieving high performance diamond-based optoelectronic devices.

FEM simulations and experimental studies of the temperature field in a large diamond crystal growth cell

We investigate the temperature field variation in the growth region of a diamond crystal in a sealed cell during the whole process of crystal growth by using the temperature gradient method （TGM） at high pressure and high temperature （HPHT）. We employ both the finite element method （FEM） and in situ experiments. Simulation results show that the temperature in the center area of the growth cell continues to decrease during the process of large diamond crystal growth. These results are in good agreement with our experimental data, which demonstrates that the finite element model can successfully predict the temperature field variations in the growth cell. The FEM simulation will be useful to grow larger high-quality diamond crystal by using the TGM. Furthermore, this method will be helpful in designing better cells and improving the growth process of gem-quality diamond crystal.

Synthesis and characterization of p-type boron-doped IIb diamond large single crystals

High-quality p-type boron-doped IIb diamond large single crystals are successfully synthesized by the temperature gradient method in a china-type cubic anvil high-pressure apparatus at about 5.5 GPa and 1600 K. The morphologies and surface textures of the synthetic diamond crystals with different boron additive quantities are characterized by using an optical microscope and a scanning electron microscope respectively. The impurities of nitrogen and boron in diamonds are detected by micro Fourier transform infrared technique. The electrical properties including resistivities, Hall coefficients, Hall mobilities and carrier densities of the synthesized samples are measured by a four-point probe and the Hall effect method. The results show that large p-type boron-doped diamond single crystals with few nitrogen impurities have been synthesized. With the increase of quantity of additive boron, some high-index crystal faces such as {113} gradually disappear, and some stripes and triangle pits occur on the crystal surface. This work is helpful for the further research and application of boron-doped semiconductor diamond.

Electrochemical Cycled Structure of MnV_2O_6 Nanoribbons Synthesized via Hydrothermal Route

1 Introduction Low-dimensional nanostructures, such as nanorods, nanowires, and nanotubes, have received much attention for their superior optical, electrical, catalytic and magnetic properties. Owing to their low dimensionality and quantum continement effect, low-dimensional nanoscale materials can be exploited as fundamental building blocks for nanoscience and nanodevices^[1-3]. In recent years, efforts have been devoted to develop new approaches to synthesize one-dimensional（lD） nanostructrued vanadium oxides or vanadates materials, such as V205, NaV2Os, and CuV206, which have been widely investigated in catalytic or electrochemical fields due to their outstanding structural flexibility^[4-6].