Solution-processing approach of nanomaterials toward an artificial sensory system

Artificial sensory systems have emerged as pivotal technologies to bridge the gap between the virtual and real-world,replicating human senses to interact intelligently with external stimuli.To practically apply artificial sensory systems in the real-world,it is essential to mass-produce nanomaterials with ensured sensitivity and selectivity,purify them for desired functions,and integrate them into large-area sensory devices through assembly techniques.A comprehensive understanding of each process parameter from material processing to device assembly is crucial for achieving a high-performing artificial sensory system.This review provides a technological framework for fabricating high-performance artificial sensory systems,covering material processing to device integrations.We introduce recent approaches for dispersing and purifying various nanomaterials including 0D,1D,and 2D nanomaterials.We then highlight advanced coating and printing techniques of the solution-processed nanomaterials based on representative three methods including(i)evaporation-based assembly,(ii)assisted assembly,and(iii)direct patterning.We explore the application and performances of these solution-processed materials and printing methods in fabricating sensory devices mimicking five human senses including vision,olfaction,gustation,hearing,and tactile perception.Finally,we suggest an outlook for possible future research directions to solve the remaining challenges of the artificial sensory systems such as ambient stability,device consistency,and integration with AI-based software.

Modification strategies improving the electrochemical and structural stability of high-Ni cathode materials

With the increasing spotlight in electric vehicles,there is a growing demand for high-energy-density batteries to enhance driving range.Consequently,several studies have been conducted on high-energy-density LiNi_(x)Co_(y)Mn_(z)O_(2)cathodes.However,there is a limit to permanent performance deterioration because of side reactions caused by moisture in the atmosphere and continuous microcracks during cycling as the Ni content to express high energy increases and the content of Mn and Co that maintain structural and electrochemical stabilization decreases.The direct modification of the surface and bulk regions aims to enhance the capacity and long-term performance of high-Ni cathode materials.Therefore,an efficient modification requires a study based on a thorough understanding of the degradation mechanisms in the surface and bulk region.In this review,a comprehensive analysis of various modifications,including doping,coating,concentration gradient,and single crystals,is conducted to solve degradation issues along with an analysis of the overall degradation mechanism occurring in high-Ni cathode materials.It also summarizes recent research developments related to the following modifications,aims to provide notable points and directions for post-studies,and provides valuable references for the commercialization of stable high-energy-density cathode materials.

Stable immobilization of lithium polysulfides using three-dimensional ordered mesoporous Mn_(2)O_(3) as the host material in lithium-sulfur batteries

Lithium-sulfur batteries(LSBs)have drawn significant attention owing to their high theoretical discharge capacity and energy density.However,the dissolution of long-chain polysulfides into the electrolyte during the charge and discharge process(“shuttle effect”)results in fast capacity fading and inferior electrochemical performance.In this study,Mn_(2)O_(3)with an ordered mesoporous structure(OM-Mn_(2)O_(3))was designed as a cathode host for LSBs via KIT-6 hard templating,to effectively inhibit the polysulfide shuttle effect.OM-Mn_(2)O_(3)offers numerous pores to confine sulfur and tightly anchor the dissolved polysulfides through the combined effects of strong polar-polar interactions,polysulfides,and sulfur chain catenation.The OM-Mn_(2)O_(3)/S composite electrode delivered a discharge capacity of 561 mAh g^(-1) after 250 cycles at 0.5 C owing to the excellent performance of OM-Mn_(2)O_(3).Furthermore,it retained a discharge capacity of 628mA h g^(-1) even at a rate of 2 C,which was significantly higher than that of a pristine sulfur electrode(206mA h g^(-1)).These findings provide a prospective strategy for designing cathode materials for high-performance LSBs.

Predictive modeling of critical temperatures in magnesium compounds using transfer learning

This study presents a transfer learning approach for discovering potential Mg-based superconductors utilizing a comprehensive target dataset.Initially,a large source dataset(Bandgap dataset)comprising approximately∼75k compounds is utilized for pretraining,followed by fine-tuning with a smaller Critical Temperature(T_(c))dataset containing∼300 compounds.Comparatively,there is a significant improvement in the performance of the transfer learning model over the traditional deep learning(DL)model in predicting Tc.Subsequently,the transfer learning model is applied to predict the properties of approximately 150k compounds.Predictions are validated computationally using density functional theory(DFT)calculations based on lattice dynamics-related theory.Moreover,to demonstrate the extended predictive capability of the transfer learning model for new materials,a pool of virtual compounds derived from prototype crystal structures from the Materials Project(MP)database is generated.T_(c) predictions are obtained for∼3600 virtual compounds,which underwent screening for electroneutrality and thermodynamic stability.An Extra Trees-based model is trained to utilize E_(hull)values to obtain thermodynamically stable materials,employing a dataset containing Ehull values for approximately 150k materials for training.Materials with Ehull values exceeding 5 meV/atom were filtered out,resulting in a refined list of potential Mg-based superconductors.This study showcases the effectiveness of transfer learning in predicting superconducting properties and highlights its potential for accelerating the discovery of Mg-based materials in the field of superconductivity.

NaF assisted preparation and the improved corrosion resistance of high content ZnO doped plasma electrolytic oxidation coating on AZ31B alloy

In the present research,the NaF assisted plasma electrolytic oxidation(PEO)is designed to fabricate the high-content ZnO nanoparti-cles doped coating on AZ31B alloy.The microstructure,phase constituents and corrosion behavior of the PEO coatings are investigated systematically.The results reveal that the introduction of NaF promotes the formation of MgF2 nanophases in the passivation layer on Mg alloy,decreasing the breakdown voltage and discharge voltage.As a result,the continuous arcing caused by high discharge voltage is alleviated.With the increasing of NaF content,the Zn content in the PEO coating is enhanced and the pore size in the coating is decreased correspondingly.Due to the high-content ZnO doping,the PEO coating protected AZ31B alloy demonstrates the better corrosion resistance.Compared with the bare AZ31B alloy,the high-content ZnO doped PEO coated sample shows an increased corrosion potential from-1.465 V to-1.008 V,a decreased corrosion current density from 3.043×10^(-5) A·cm^(-2) to 3.960×10^(-8) A·cm^(-2) and an increased charge transfer resistance from 1.213×10^(2) ohm·cm^(2) to 2.598×10^(5) ohm·cm^(2).Besides,the high-content ZnO doped PEO coated sample also has the excellent corrosion resistance in salt solution,exhibiting no obvious corrosion after more than 2000 h neutral salt spraying and 28 days’immersion testing.The improved corrosion resistance can be ascribed to the relative uniform distribution of ZnO in PEO coating which can transform to Zn(OH)2 and form a continuous protective layer along the corrosion interface.

Low-firing and temperature stability regulation of tri-rutile MgTa_(2)O_(6)microwave dielectric ceramics

A glass frit containing Li_(2)O-MgO-ZnO-B_(2)O_(3)-SiO_(2)component was used to explore the low-temperature sintering behaviors and microwave dielectric characteristics of tri-rutile MgTa_(2)O_(6)ceramics in this study.The good low-firing effects are presented due to the high matching relevance between Li_(2)O-MgO-ZnO-B_(2)O_(3)-SiO_(2)glass and MgTa_(2)O_(6)ceramics.The pure tri-rutile MgTa_(2)O_(6)structure remains unchanged,and high sintering compactness can also be achieved at 1150℃.We found that the Li_(2)O-MgO-ZnO-B_(2)O_(3)-SiO_(2)glass not only greatly improves the low-temperature sintering characteristics of MgTa_(2)O_(6)ceramics but also maintains a high(quality factor(Q)×resonance frequency(f))value while still improving the temperature stability.Typically,great microwave dielectric characteristics when added with 2wt%Li_(2)O-MgO-ZnO-B_(2)O_(3)-SiO_(2)glass can be achieved at 1150℃:dielectric constant,ε_(r)=26.1;Q×f=34267 GHz;temperature coefficient of resonance frequency,τ_(f)=-8.7×10^(-6)/℃.

Sand control mechanism of radial well filled with phase change material in hydrate reservoir

Radial well filled with phase change material has been proposed as a novel sand control method for hydrate exploitation.In order to reveal the sand control mechanism,CFD-DEM coupling method is applied to simulate the migration,settlement,and blockage processes of sand particles in the radial well.The obtained results indicate that three scenarios have been recognized for sand particles passing through sand control medium,based on the diameter ratio of sand control medium to sand particle(D_(d)):fully passing(D_(d)=8.75-22.5),partially passing and partially blocked(D_(d)=3.18-5.63),and completely blocked(D_(d)=2.18-3.21).After being captured by the sand control medium,sand particles can block pores,which increases fluid flow resistance and causes a certain pressure difference in the radial well.The pressure in the radial well should be lower than the hydrate phase equilibrium pressure during sand control design,for the purpose of promoting hydrate decomposition,and sand capture.The length of the radial well should be optimized based on the reservoir pore pressure,production pressure difference,bottom hole pressure,and the pressure gradient in the radial well.It should be noticed that the sand control medium leads to a decrease in permeability after sand particles captured.Even the permeability is reduced to several hundred millidarcy,it is still sufficient to ensure the effective flow of gas and water after hydrate decomposition.Increasing fluid velocity reduces the blocking capacity of the sand control medium,mainly because of deterioration in bridging between sand particles.

Progress of Materials and Devices for Neuromorphic Vision Sensors

The latest developments in bio-inspired neuromorphic vision sensors can be summarized in 3 keywords:smaller,faster,and smarter.(1)Smaller:Devices are becoming more compact by integrating previously separated components such as sensors,memory,and processing units.As a prime example,the transition from traditional sensory vision computing to in-sensor vision computing has shown clear benefits,such as simpler circuitry,lower power consumption,and less data redundancy.(2)Swifter:Owing to the nature of physics,smaller and more integrated devices can detect,process,and react to input more quickly.In addition,the methods for sensing and processing optical information using various materials(such as oxide semiconductors)are evolving.(3)Smarter:Owing to these two main research directions,we can expect advanced applications such as adaptive vision sensors,collision sensors,and nociceptive sensors.This review mainly focuses on the recent progress,working mechanisms,image pre-processing techniques,and advanced features of two types of neuromorphic vision sensors based on near-sensor and in-sensor vision computing methodologies.

Thermodynamically Revealing the Essence of Order and Disorder Structures in Layered Cathode Materials

Layered transition metal(TM) oxides are one of the most widely used cathode materials in lithium-ion batteries. The atomic configuration in TM layer of these materials is often known to be random when multiple TM elements co-exist in the layer(e.g. Ni, Co and Mn). By contrast, the configuration tends to be ordered if the elements are Li and Mn. Here, by using special quasi-random structures(SQS) algorithm, the essential reasons of the ordering in a promising Li-rich Mn-based cathode material Li2MnO3 are investigated. The difference of internal energy and entropy between ordered and disordered materials is calculated. As a result, based on the Gibbs free energy, it is found that Li2MnO3 should have an ordered structure in TM layer. In comparison, structures with Ni-Mn ratio of 2:1 are predicted to have a disordered TM layer, because the entropy terms have larger impact on the structural ordering than internal energy terms.

Practical evaluation of prelithiation strategies for next-generation lithium-ion batteries

With the increasing market demand for high-performance lithium-ion batteries with high-capacity electrode materials,reducing the irreversible capacity loss in the initial cycle and compensating for the active lithium loss during the cycling process are critical challenges.In recent years,various prelithiation strategies have been developed to overcome these issues.Since these approaches are carried out under a wide range of conditions,it is essential to evaluate their suitability for large-scale commercial applications.In this review,these strategies are categorized based on different battery assembling stages that they are implemented in,including active material synthesis,the slurry mixing process,electrode pretreatment,and battery fabrication.Furthermore,their advantages and disadvantages in commercial production are discussed from the perspective of thermodynamics and kinetics.This review aims to provide guidance for the future development of prelithiation strategies toward commercialization,which will potentially promote the practical application of next-generation high-energy-density lithium-ion batteries.

Atomic layer deposition of thin films:from a chemistry perspective

Atomic layer deposition(ALD)has become an indispensable thin-film technology in the contemporary microelectronics industry.The unique self-limited layer-by-layer growth feature of ALD has outstood this technology to deposit highly uniform conformal pinhole-free thin films with angstrom-level thickness control,particularly on 3D topologies.Over the years,the ALD technology has enabled not only the successful downscaling of the microelectronic devices but also numerous novel 3D device structures.As ALD is essentially a variant of chemical vapor deposition,a comprehensive understanding of the involved chemistry is of crucial importance to further develop and utilize this technology.To this end,we,in this review,focus on the surface chemistry and precursor chemistry aspects of ALD.We first review the surface chemistry of the gas–solid ALD reactions and elaborately discuss the associated mechanisms for the film growth;then,we review the ALD precursor chemistry by comparatively discussing the precursors that have been commonly used in the ALD processes;and finally,we selectively present a few newly-emerged applications of ALD in microelectronics,followed by our perspective on the future of the ALD technology.

Solvent-free fabrication of broadband WS2 photodetectors on paper

Paper-based devices have attracted extensive attention due to the growing demand for disposable flexible electronics.Herein,we integrate semiconducting devices on cellulose paper substrate through a simple abrasion technique that yields high-performance photodetectors.A solvent-free WS_(2) film deposited on paper favors an effective electron-hole separation and hampers recombination.The as-prepared paper-based WS2 photodetectors exhibit a sensitive photoresponse over a wide spectral range spanning from ultraviolet(365 nm)to near-infrared(940 nm).Their responsivity value reaches up to~270 mA W^(−1) at 35 V under a power density of 35 mW cm^(−2).A high performance photodetector was achieved by controlling the environmental exposure as the ambient oxygen molecules were found to decrease the photoresponse and stability of the WS_(2) photodetector.Furthermore,we have built a spectrometer using such a paperbased WS_(2) device as the photodetecting component to illustrate its potential application.The present work could promote the development of cost-effective disposable photodetection devices.

The mechanism of external pressure suppressing dendrites growth in Li metal batteries

Li metal is considered an ideal anode material for application in the next-generation secondary batteries.However,the commercial application of Li metal batteries has not yet been achieved due to the safety concern caused by Li dendrites growth.Despite the fact that many recent experimental studies found that external pressure suppresses the Li dendrites growth,the mechanism of the external pressure effect on Li dendrites remains poorly understood on the atomic scale.Herein,the large-scale molecular dynamics simulations of Li dendrites growth under different external pressure were performed with a machine learning potential,which has the quantum-mechanical accuracy.The simulation results reveal that the external pressure promotes the process of Li self-healing.With the increase of external pressure,the hole defects and Li dendrites would gradually fuse and disappear.This work provides a new perspective for understanding the mechanism for the impact of external pressure on Li dendrites.

Brittle and ductile characteristics of intermetallic compounds in magnesium alloys: A large-scale screening guided by machine learning

In the present work,we have employed machine learning(ML)techniques to evaluate ductile-brittle(DB)behaviors in intermetallic compounds(IMCs)which can form magnesium(Mg)alloys.This procedure was mainly conducted by a proxy-based method,where the ratio of shear(G)/bulk(B)moduli was used as a proxy to identify whether the compound is ductile or brittle.Starting from compounds information(composition and crystal structure)and their moduli,as found in open databases(AFLOW),ML-based models were built,and those models were used to predict the moduli in other compounds,and accordingly,to foresee the ductile-brittle behaviors of these new compounds.The results reached in the present work showed that the built models can effectively catch the elastic moduli of new compounds.This was confirmed through moduli calculations done by density functional theory(DFT)on some compounds,where the DFT calculations were consistent with the ML prediction.A further confirmation on the reliability of the built ML models was considered through relating between the DB behavior in MgBe_(13) and MgPd_(2),as evaluated by the ML-predicted moduli,and the nature of chemical bonding in these two compounds,which in turn,was investigated by the charge density distribution(CDD)and electron localization function(ELF)obtained by DFT methodology.The ML-evaluated DB behaviors of the two compounds was also consistent with the DFT calculations of CDD and ELF.These findings and confirmations gave legitimacy to the built model to be employed in further prediction processes.Indeed,as examples,the DB characteristics were investigated in IMCs that might from in three Mg alloy series,involving AZ,ZX and WE.

A rational preparation strategy of phase tuned MoO_(3) nanostructures for high-performance all-solid asymmetric supercapacitor

In this work,phase and morphology-tuned MoO_(3) nanostructures are synthesized through a novel modified co-precipitation method,and their electrochemical properties are investigated.For the first time,such a simple surfactant-assisted synthesis process aided by minor temperature variations is reported which results in phase transition of the nanoparticles from h-MoO_(3) nano-rods to a-MoO_(3) nano-flakes.The nanostructures thus developed are highly porous and crystalline with significantly large specific surface area as compared to previous literature.The theoretical bandgap energy of the optimized sample calculated using Perdew-Zunger local density approximation(LDA) is in good agreement with the experimental findings.An overall structural,morphological,and surface-behavioural analysis predicts the electrochemical superiority in 2D a-MoO_(3).The cyclic voltammetry and galvano-potentiometry measurements of 2D a-MoO_(3) in the potential window of-0.6 V to +0.2 V present the highest pseudosupercapacitive response with a maximum specific capacitance of 829 F g^(-1)at 2 A g^(-1)as compared to h-MoO_(3) (452 F g^(-1)) and h@a-MoO_(3) (783 F g^(-1)).Thus,the MoO_(3) 2D nanostructures synthesized through our novel synthesis technique display excellent specific capacitance as compared to previous reported data.Additionally,a-MoO_(3) exhibits a galvanostatic charging-discharging cyclic stability of about 91%after 2000 cycles,indicating that it can serve as an excellent electrode material for supercapacitors.A solid-state asymmetric supercapacitor device is successfully constructed using a-MoO_(3) which can light up 4 red LEDs for 10 s.The specific energy density of the device reaches a maximum value of 36.3 W h kg^(-1)at the power density of 50 W kg^(-1).

Synergically enhanced piezocatalysis performance of eco-friendly(K_(0.52)Na_(0.48))NbO_(3) through ferroelectric polarization and defects

Piezocatalysis has attracted unprecedented research interest as a newly emerging catalysis technology.However,the inherent insulating property of ferroelectric materials ultimately leads to the poor vibration-electricity conversion ability.Herein,this work reports the(K_(0.52)Na_(0.48))NbO_(3) ferroelectric ceramics(KNNFCx),for which the FeCo modification strategy is proposed.The substitution of the moderate amount of FeCo(x=0.015)at Nb site not only optimizes ferroelectricity but also produces beneficial defects,notably increasing Rhodamine B water purification efficiency to 95%.The pinning effect of monovalent oxygen vacancies on ferroelectric domains is responsible for the excellent ferroelectric polarization of KNNFC0.015 through the generation of an internal field to promote charge carriers separation and reduce nonradiative recombination.Importantly,the accompanying electron carriers can easily move to the material surface and participate in redox reactions because they have low activation energy.Therefore,ferroelectric polarization and defects play synergetic roles in enhancing piezocatalytic performance.

Clarification of underneath capacity loss for O3-type Ni, co free layered cathodes at high voltage for sodium ion batteries

Earth abundant O3-type NaFe_(0.5)Mn_(0.5)O_(2)layered oxide is regarded as one of the most promising cathodes for sodium ion batteries due to its low cost and high energy density.However,its poor structural stability and cycle life strongly impede the practical application.Herein,the dynamic phase evolution as well as charge compensation mechanism of O3-type NaFe_(0.5)Mn_(0.5)O_(2)cathode during sodiation/desodiation are revealed by a systemic study with operando X-ray diffraction and X-ray absorption spectroscopy,high resolution neutron powder diffraction and neutron pair distribution functions.The layered structure experiences a phase transition of O3→P3→OP2→ramsdellite during the desodiation,and a new O3’phase is observed at the end of the discharge state(1.5 V).The density functional theory(DFT)calculations and nPDF results suggest that depletion of Na^(+)ions induces the movement of Fe into Na layer resulting the formation of an inert ramsdellite phase thus causing the loss of capacity and structural integrity.Meanwhile,the operando XAS clarified the voltage regions for active Mn^(3+)/Mn^(4+)and Fe^(3+)/Fe^(4+)redox couples.This work points out the universal underneath problem for Fe-based layered oxide cathodes when cycled at high voltage and highlights the importance to suppress Fe migration regarding the design of high energy O3-type cathodes for sodium ion batteries.

A semi-classical model for the charge exchange and energy loss of slow highly charged ions in ultrathin materials

We present a simple and reliable method,based on the over-barrier model and Lindhard’s formula,to calculate the energy loss,charge transfer,and normalized intensity of highly charged ions penetrating through 2D ultrathin materials,including graphene and carbon nanomembranes.According to our results,the interaction between the ions and the 2D material can be simplified as an equivalent two-body collision,and we find that full consideration of the charge exchange effect is key to understanding the mechanism of ion energy deposition in an ultrathin target.Not only can this semiclassical model be used to evaluate the ion irradiation effect to a very good level of accuracy,but it also provides important guidance for tailoring the properties of 2D materials using ion beams.

Improved RF power performance of InAlN/GaN HEMT by optimizing rapid thermal annealing process for high-performance low-voltage terminal applications

Improved radio-frequency(RF)power performance of InAlN/GaN high electron mobility transistor(HEMT)is achieved by optimizing the rapid thermal annealing(RTA)process for high-performance low-voltage terminal applications.By optimizing the RTA temperature and time,the optimal annealing condition is found to enable low parasitic resistance and thus a high-performance device.Besides,compared with the non-optimized RTA HEMT,the optimized one demonstrates smoother ohmic metal surface morphology and better heterojunction quality including the less degraded heterojunction sheet resistance and clearer heterojunction interfaces as well as negligible material out-diffusion from the barrier to the channel and buffer.Benefiting from the lowered parasitic resistance,improved maximum output current density of 2279 mA·mm^(-1)and higher peak extrinsic transconductance of 526 mS·mm^(-1)are obtained for the optimized RTA HEMT.In addition,due to the superior heterojunction quality,the optimized HEMT shows reduced off-state leakage current of 7×10^(-3)mA·mm^(-1)and suppressed current collapse of only 4%,compared with those of 1×10^(-1)mA·mm^(-1)and 15%for the non-optimized one.At 8 GHz and V_(DS)of 6 V,a significantly improved power-added efficiency of 62%and output power density of 0.71 W·mm^(-1)are achieved for the optimized HEMT,as the result of the improvement in output current,knee voltage,off-state leakage current,and current collapse,which reveals the tremendous advantage of the optimized RTA HEMT in high-performance low-voltage terminal applications.

A study of highly activated hydrogen evolution reaction performance in acidic media by 2D heterostructure of N and S doped graphene on MoO_(x)

Herein,a layer of molybdenum oxide(MoO_(x)),a transition metal oxide(TMO),which has outstanding catalytic properties in combination with a carbonbased thin film,is modified to improve the hydrogen production performance and protect the MoO_(x)in acidic media.A thin film of graphene is transferred onto the MoO_(x)layer,after which the graphene structure is doped with N and S atoms at room temperature using a plasma doping method to modify the electronic structure and intrinsic properties of the material.The oxygen functional groups in graphene increase the interfacial interactions and electrical contacts between graphene and MoO_(x).The appearance of surface defects such as oxygen vacancies can result in vacancies in MoO_(x).This improves the electrical conductivity and electrochemically accessible surface area.Increasing the number of defects in graphene by adding dopants can significantly affect the chemical reaction at the interfaces and improve the electrochemical performance.These defects in graphene play a crucial role in the adsorption of H^(+)ions on the graphene surface and their transport to the MoO_(x)layer underneath.This enables MoO_(x)to participate in the reaction with the doped graphene.N^(‐)and S^(‐)doped graphene(NSGr)on MoO_(x)is active in acidic media and performs well in terms of hydrogen production.The initial overpotential value of 359 mV for the current density of−10 mA/cm^(2)is lowered to 228 mV after activation.