Recent Advances in In-Memory Computing:Exploring Memristor and Memtransistor Arrays with 2D Materials

The conventional computing architecture faces substantial chal-lenges,including high latency and energy consumption between memory and processing units.In response,in-memory computing has emerged as a promising alternative architecture,enabling computing operations within memory arrays to overcome these limitations.Memristive devices have gained significant attention as key components for in-memory computing due to their high-density arrays,rapid response times,and ability to emulate biological synapses.Among these devices,two-dimensional(2D)material-based memristor and memtransistor arrays have emerged as particularly promising candidates for next-generation in-memory computing,thanks to their exceptional performance driven by the unique properties of 2D materials,such as layered structures,mechanical flexibility,and the capability to form heterojunctions.This review delves into the state-of-the-art research on 2D material-based memristive arrays,encompassing critical aspects such as material selection,device perfor-mance metrics,array structures,and potential applications.Furthermore,it provides a comprehensive overview of the current challenges and limitations associated with these arrays,along with potential solutions.The primary objective of this review is to serve as a significant milestone in realizing next-generation in-memory computing utilizing 2D materials and bridge the gap from single-device characterization to array-level and system-level implementations of neuromorphic computing,leveraging the potential of 2D material-based memristive devices.

Microwave shock motivating the Sr substitution of 2D porous GdFeO_(3) perovskite for highly active oxygen evolution

The incorporation of partial A-site substitution in perovskite oxides represents a promising strategy for precisely controlling the electronic configuration and enhancing its intrinsic catalytic activity.Conventional methods for A-site substitution typically involve prolonged high-temperature processes.While these processes promote the development of unique nanostructures with highly exposed active sites,they often result in the uncontrolled configuration of introduced elements.Herein,we present a novel approach for synthesizing two-dimensional(2D)porous GdFeO_(3) perovskite with A-site strontium(Sr)substitution utilizing microwave shock method.This technique enables precise control of the Sr content and simultaneous construction of 2D porous structures in one step,capitalizing on the advantages of rapid heating and cooling(temperature~1100 K,rate~70 K s^(-1)).The active sites of this oxygen-rich defect structure can be clearly revealed through the simulation of the electronic configuration and the comprehensive analysis of the crystal structure.For electrocatalytic oxygen evolution reaction application,the synthesized 2D porous Gd_(0.8)Sr_(0.2)FeO_(3) electrocatalyst exhibits an exceptional overpotential of 294 mV at a current density of 10 mA cm^(-2)and a small Tafel slope of 55.85 mV dec^(-1)in alkaline electrolytes.This study offers a fresh perspective on designing crystal configurations and the construction of nanostructures in perovskite.

Understanding the oxidation chemistry of Ti_(3)C_(2)T_(x)(MXene)sheets and their catalytic performances

Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.

2D multifunctional devices:from material preparation to device fabrication and neuromorphic applications

Neuromorphic computing systems,which mimic the operation of neurons and synapses in the human brain,are seen as an appealing next-generation computing method due to their strong and efficient computing abilities.Two-dimensional (2D) materials with dangling bond-free surfaces and atomic-level thicknesses have emerged as promising candidates for neuromorphic computing hardware.As a result,2D neuromorphic devices may provide an ideal platform for developing multifunctional neuromorphic applications.Here,we review the recent neuromorphic devices based on 2D material and their multifunctional applications.The synthesis and next micro–nano fabrication methods of 2D materials and their heterostructures are first introduced.The recent advances of neuromorphic 2D devices are discussed in detail using different operating principles.More importantly,we present a review of emerging multifunctional neuromorphic applications,including neuromorphic visual,auditory,tactile,and nociceptive systems based on 2D devices.In the end,we discuss the problems and methods for 2D neuromorphic device developments in the future.This paper will give insights into designing 2D neuromorphic devices and applying them to the future neuromorphic systems.

Patterning single-layer materials by electrical breakdown using atomic force microscopy

The development of nanoelectronics and nanotechnologies has been boosted significantly by the emergence of 2D materials because of their atomic thickness and peculiar properties,and developing a universal,precise patterning technology for single-layer 2D materials is critical for assembling nanodevices.Demonstrated here is a nanomachining technique using electrical breakdown by an AFM tip to fabricate nanopores,nanostrips,and other nanostructures on demand.This can be achieved by voltage scanning or applying a constant voltage while moving the tip.By measuring the electrical current,the formation process on single-layer materials was shown quantitatively.The present results provide evidence of successful pattern fabrication on single-layer MoS2,boron nitride,and graphene,although further confirmation is still needed.The proposed method holds promise as a general nanomachining technology for the future.

Microwave-assisted exploration of the electron configuration-dependent electrocatalytic urea oxidation activity of 2D porous NiCo_(2)O_(4) spinel

Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spinel synthesis methods with prolonged high-temperature reactions lack kinetic precision,hindering the balance between controlled doping and highly active two-dimensional(2D)porous structures design.This significantly impedes the identification of electron configuration-dependent active sites in doped 2D nickel-based spinels.Herein,we present a microwave shock method for the preparation of 2D porous NiCo_(2)O_(4)spinel.Utilizing the transient on-off property of microwave pulses for precise heteroatom doping and 2D porous structural design,non-metal doping(boron,phosphorus,and sulfur)with distinct extranuclear electron disparities serves as straightforward examples for investigation.Precise tuning of lattice parameter reveals the impact of covalent bond strength on NiCo_(2)O_(4)structural stability.The introduced defect levels induce unpaired d-electrons in transition metals,enhancing the adsorption of electron-donating amino groups in urea molecules.Simultaneously,Bode plots confirm the impact mechanism of rapid electron migration caused by reduced band gaps on UOR activity.The prepared phosphorus-doped 2D porous NiCo_(2)O_(4),with optimal electron configuration control,outperforms most reported spinels.This controlled modification strategy advances understanding theoretical structure-activity mechanisms of high-performance 2D spinels in UOR.

MXenes: Versatile 2D materials with tailored surface chemistry and diverse applications

MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical strength,etc.This review begins by presenting MXenes,providing insights into their structural characteristics,synthesis methods,and surface functional groups.The review covers a thorough analysis of MXene surface properties,including surface chemistry and termination group impacts.The properties of MXenes are influenced by their synthesis,which can be fluorine-based or fluorinedependent.Fluorine-based synthesis techniques involve etching with fluorine-based reagents,mainly including HF or LiF/HCl,while fluorine-free methods include electrochemical etching,chemical vapor deposition(CVD),alkaline etching,Lewis acid-based etching,etc.These techniques result in the emergence of functional groups such as-F,-O,-OH,-Cl,etc.on the MXenes surface,depending on the synthesis method used.Properties of MXenes,such as electrical conductivity,electronic properties,catalytic activity,magnetic properties,mechanical strength,and chemical and thermal stability,are examined,and the role of functional groups in determining these properties is explored.The review delves into the diverse applications of MXenes,encompassing supercapacitors,battery materials,hydrogen storage,fuel cells,electromagnetic interference(EMI) shielding,pollutant removal,water purification,flexible electronics,sensors,additive manufacturing,catalysis,biomedical and healthcare fields,etc.Finally,this article outlines the challenges and opportunities in the current and future development of MXenes research,addressing various aspects such as synthesis scalability,etching challenges,and multifunctionality,and exploring novel applications.The review concludes with future prospects and conclusions envisioning the impact of MXenes on future technologies and innovation.

Electrocatalytic stability of two-dimensional materials

In electrocatalysis,two-dimensional(2D)materials have attracted extensive interests due to their unique electronic structure and physical properties.In recent years,many efforts have been devoted to improving the catalytic activity of 2D materials.However,the stability of 2D materials under catalytic conditions,as a critical issue,requires better understanding for any practical applications.This review summarizes recent progress in electrocatalytic stability of 2D materials,including four intrinsic factors that affect the stability of 2D materials:1.Weak interactions between 2D catalyst and substrate;2,delamination of 2D catalyst layers;3.metastable phase of 2D materials;4.chemistry and environmental instability of 2D materials.Meanwhile,some corresponding solutions are summarized for each factor.In addition,this review proposes potential routes for developing 2D catalytic materials with both high activity and stability.

Two-dimensional MOF-based materials:Preparations and applications as electrodes in Li-ion batteries

Two-dimensional(2D)metal-organic frameworks(MOFs)are rapidly emerging as a unique class of mushrooming family of 2D materials offering distinctive features,such as hierarchical porosity,extensive surface area,easily available active sites,and versatile,adaptable structures.These promising characteristics have positioned them as highly appealing alternatives for a wide range of applications in energy storage technologies,including lithium batteries.Nevertheless,the poor conductivity and limited stability of 2D MOFs have limited their real applications in electrochemical energy storage.These limitations have therefore warranted ongoing research to enhance the performance of 2D MOFs.Given the significance of 2D MOF-based materials as an emerging class of advanced materials,a multitude of strategy has been devised to address these challenges such as synthesizing 2D conductive MOFs and derivatives along with 2D MOF hybridization.One promising approach involves the use of 2D MOF derivatives,including transition metal oxides,which due to their abundant unsatu rated active metal sites and shorter diffusion paths,offer superior electrochemical performance.Additionally,by combining pristine 2D MOFs with other materials,hybrid 2D MOF materials can be created.These hybrids,with their enhanced stability and conductivity,can be directly utilized as active materials in lithium batteries.In the present review,we categorize 2D MOF-based materials into three distinct groups:pristine 2D MOFs,2D MOFderived materials,and 2D MOF hybrid materials.The synthesis methods for each group,along with their specific applications as electrode materials in lithium-ion batteries,are discussed in detail.This comprehensive review provides insights into the potential of 2D MOFs while highlighting the opportunities and challenges that are present in this evolving field.

Electronic properties of 2D materials and their junctions

With an extensive range of distinctive features at nano meter-scale thicknesses,two-dimensional(2D)materials drawn the attention of the scientific community.Despite tremendous advancements in exploratory research on 2D materials,knowledge of 2D electrical transport and carrier dynamics still in its infancy.Thus,here we highlighted the electrical characteristics of 2D materials with electronic band structure,electronic transport,dielectric constant,carriers mobility.The atomic thinness of 2D materials makes substantially scaled field-effect transistors(FETs)with reduced short-channel effects conceivable,even though strong carrier mobility required for high performance,low-voltage device operations.We also discussed here about factors affecting 2D materials which easily enhanced the activity of those materials for various applications.Presently,Those 2D materials used in state-of-the-art electrical and optoelectronic devices because of the extensive nature of their electronic band structure.2D materials offer unprecedented freedom for the design of novel p-n junction device topologies in contrast to conventional bulk semiconductors.We also,describe the numerous 2D p-n junctions,such as homo junction and hetero junction including mixed dimensional junctions.Finally,we talked about the problems and potential for the future.

M_(4)X_(3) MXenes:Application in Energy Storage Devices

MXene has garnered widespread recognition in the scientific com-munity due to its remarkable properties,including excellent thermal stability,high conductivity,good hydrophilicity and dispersibility,easy processability,tunable surface properties,and admirable flexibility.MXenes have been categorized into different families based on the number of M and X layers in M_(n+1)X_(n),such as M_(2)X,M_(3)X_(2),M_(4)X_(3),and,recently,M_(5)X_(4).Among these families,M_(2)X and M_(3)X_(2),par-ticularly Ti_(3)C_(2),have been greatly explored while limited studies have been given to M_(5)X_(4)MXene synthesis.Meanwhile,studies on the M_(4)X_(3)MXene family have developed recently,hence,demanding a compilation of evaluated studies.Herein,this review provides a systematic overview of the latest advancements in M_(4)X_(3)MXenes,focusing on their properties and applications in energy storage devices.The objective of this review is to provide guidance to researchers on fostering M_(4)X_(3)MXene-based nanomaterials,not only for energy storage devices but also for broader applications.

Fabrication and applications of van der Waals heterostructures

Van der Waals heterostructures(vdWHs) are showing considerable potential in both fundamental exploration and practical applications. Built upon the synthetic successes of(two-dimensional) 2D materials, several synthetic strategies of vdWHs have been developed,allowing the convenient fabrication of diverse vdWHs with decent controllability, quality, and scalability. This review first summarizes the current state of the art in synthetic strategies of vdWHs, including physical combination, deposition, solvothermal synthesis, and synchronous evolution. Then three major applications and their representative vdWH devices have been reviewed, including electronics(tunneling field effect transistors and 2D contact),optoelectronics(photodetector), and energy conversion(electrocatalysts and metal ion batteries), to unveil the potentials of vdWHs in practical applications and provide the general design principles of functional vdWHs for different applications. Besides, moiré superlattices based on vdWHs are discussed to showcase the importance of vdWHs as a platform for novel condensed matter physics. Finally, the crucial challenges towards ideal vdWHs with high performance are discussed, and the outlook for future development is presented. By the systematical integration of synthetic strategies and applications, we hope this review can further light up the rational designs of vdWHs for emerging applications.

Switching of K-Q intervalley trions fine structure and their dynamics in n-doped monolayer WS_(2)

Monolayer group VI transition metal dichalcogenides(TMDs)have recently emerged as promising candidates for photonic and opto-valleytronic applications.The optoelectronic properties of these atomically-thin semiconducting crystals are strongly governed by the tightly bound electron-hole pairs such as excitons and trions(charged excitons).The anomalous spin and valley configurations at the conduction band edges in monolayer WS_(2)give rise to even more fascinating valley many-body complexes.Here we find that the indirect Q valley in the first Brillouin zone of monolayer WS_(2)plays a critical role in the formation of a new excitonic state,which has not been well studied.By employing a high-quality h-BN encapsulated WS_(2)field-effect transistor,we are able to switch the electron concentration within K-Q valleys at conduction band edges.Consequently,a distinct emission feature could be excited at the high electron doping region.Such feature has a competing population with the K valley trion,and experiences nonlinear power-law response and lifetime dynamics under doping.Our findings open up a new avenue for the study of valley many-body physics and quantum optics in semiconducting 2D materials,as well as provide a promising way of valley manipulation for next-generation entangled photonic devices.

Multilayered PdTe_(2)/thin Si heterostructures as self-powered flexible photodetectors with heart rate monitoring ability

Two-dimensional layered material/semiconductor heterostructures have emerged as a category of fascinating architectures for developing highly efficient and low-cost photodetection devices.Herein,we present the construction of a highly efficient flexible light detector operating in the visible-near infrared wavelength regime by integrating a PdTe2 multilayer on a thin Si film.A representative device achieves a good photoresponse performance at zero bias including a sizeable current on/off ratio exceeding 105,a decent responsivity of~343 mA/W,a respectable specific detectivity of~2.56×10^(12)Jones,and a rapid response time of 4.5/379μs,under 730 nm light irradiation.The detector also displays an outstanding long-term air stability and operational durability.In addition,thanks to the excellent flexibility,the device can retain its prominent photodetection performance at various bending radii of curvature and upon hundreds of bending tests.Furthermore,the large responsivity and rapid response speed endow the photodetector with the ability to accurately probe heart rate,suggesting a possible application in the area of flexible and wearable health monitoring.

Deep Learning Accelerates the Discovery of Two- Dimensional Catalysts for Hydrogen Evolution Reaction

Two-dimensional materials with active sites are expected to replace platinum as large-scale hydrogen production catalysts.However,the rapid discovery of excellent two-dimensional hydrogen evolution reaction catalysts is seriously hindered due to the long experiment cycle and the huge cost of high-throughput calculations of adsorption energies.Considering that the traditional regression models cannot consider all the potential sites on the surface of catalysts,we use a deep learning method with crystal graph convolutional neural networks to accelerate the discovery of high-performance two-dimensional hydrogen evolution reaction catalysts from two-dimensional materials database,with the prediction accuracy as high as 95.2%.The proposed method considers all active sites,screens out 38 high performance catalysts from 6,531 two-dimensional materials,predicts their adsorption energies at different active sites,and determines the potential strongest adsorption sites.The prediction accuracy of the two-dimensional hydrogen evolution reaction catalysts screening strategy proposed in this work is at the density-functional-theory level,but the prediction speed is 10.19 years ahead of the high-throughput screening,demonstrating the capability of crystal graph convolutional neural networks-deep learning method for efficiently discovering high-performance new structures over a wide catalytic materials space.

Computational design of promising 2D electrode materials for Li-ion and Li–S battery applications

Lithium-ion batteries(LIBs)and lithium-sulfur(Li–S)batteries are two types of energy storage systems with significance in both scientific research and commercialization.Nevertheless,the rational design of electrode materials for overcoming the bottlenecks of LIBs and Li–S batteries(such as low diffusion rates in LIBs and low sulfur utilization in Li–S batteries)remain the greatest challenge,while two-dimensional(2D)electrodes materials provide a solution because of their unique structural and electrochemical properties.In this article,from the perspective of ab-initio simulations,we review the design of 2D electrode materials for LIBs and Li–S batteries.We first propose the theoretical design principles for 2D electrodes,including stability,electronic properties,capacity,and ion diffusion descriptors.Next,classified examples of promising 2D electrodes designed by theoretical simulations are given,covering graphene,phosphorene,MXene,transition metal sulfides,and so on.Finally,common challenges and a future perspective are provided.This review paves the way for rational design of 2D electrode materials for LIBs and Li–S battery applications and may provide a guide for future experiments.

Wetting of MXenes and Beyond

MXenes are a class of 2D nanomaterials with exceptional tailormade properties such as mechano-ceramic nature,rich chemistry,and hydrophilicity,to name a few.However,one of the most challenging issues in any composite/hybrid system is the interfacial wetting.Having a superior integrity of a given composite system is a direct consequence of the proper wettability.While wetting is a fundamental feature,dictating many physical and chemical attributes,most of the common nanomaterials possesses poor affinity due to hydrophobic nature,making them hard to be easily dispersed in a given composite.Thanks to low contact angle,MXenes can offer themselves as an ideal candidate for manufacturing different nano-hybrid structures.Herein this review,it is aimed to particularly study the wettability of MXenes.In terms of the layout of the present study,MXenes are first briefly introduced,and then,the wettability phenomenon is discussed in detail.Upon reviewing the sporadic research efforts conducted to date,a particular attention is paid on the current challenges and research pitfalls to light up the future perspectives.It is strongly believed that taking the advantage of MXene’s rich hydrophilic surface may have a revolutionizing role in the fabrication of advanced materials with exceptional features.

2D Janus polymer nanosheets for enhancing oil recovery:From material ppreparation to property evaluation

Janus amphiphilic polymer nanosheets(JAPNs)with anisotropic morphology and distinctive perfor-mance have aroused widespread interest.However,due to the difficulty in synthesis and poor dispersion stability,JAPNs have been scarcely reported in the field of enhancing oil recovery(EOR).Herein,a kind of organic-based flexible JAPNs was prepared by paraffin emulsion methods.The lateral sizes of JAPNs were ranging from hundreds of nanometers to several micrometers and the thickness was about 3 nm.The organic-based nanosheets were equipped with remarkably flexible structures,which could improve their injection performance.The dispersion and interfacial properties of JAPNs were studied systematically.By modification of crosslinking agent containing multiple amino groups,the JAPNs had excellent hydro-philicity and salt resistance compared with conventional inorganic or composite nanosheets.The settling time of nanosuspension with NaCl and CaCl_(2) at a low salinity of 1000 mg/L was over 240 h.The value could also remain 124 h under the salinity of 10,000 mg/L NaCl.With the dual functionalities of Janus amphiphilic nature and nanoparticles'Pickering effect,JAPNs could change rock wettability and form emulsions as"colloidal surfactants",In particular,a new technology called optical microrheology was pioneered to explore the destabilization state of nanosuspensions for the first time.Since precipitation lagged behind aggregation,especially for stable suspension systems,the onset of the unstable behavior was difficult to be detected by conventional methods,which should be the indicator of reduced effec-tiveness for nanofluid products.In addition,the oil displacement experiments demonstrated that the JAPNs could enhance oil recovery by 17.14%under an ultra-low concentration of 0.005%and were more suitable for low permeability cores.The findings can help for a better understanding of the material preparation of polymer nanosheets.We also hope that this study could shed more light on the nano-flooding technology for EOR.

MXene:From synthesis to environment remediation

A new burgeoning family of two-dimensional(2D)transition metal carbides/nitrides,better known as MXenes,have received extensive attention because of their distinct properties,such as metallic conductivity,good hydrophilicity,large surface area,good mechanical stability,and biodegradability.About 40 different MXenes have been synthesized,and dozens more structures and properties have been theoretically predicted.However,the recent progress in MXenes development is not well covered in chronological order based on different applications.This review article focuses on emerging synthesis methods,the properties of MXenes,and mainly the applications of MXenes and MXene-based material family in environmental remediation,a comprehensive review of gaseous and aqueous pollutants treatment.

2D Materials Boost Advanced Zn Anodes:Principles,Advances,and Challenges

Aqueous zinc-ion battery(ZIB)featuring with high safety,low cost,environmentally friendly,and high energy density is one of the most promising systems for large-scale energy storage application.Despite extensive research progress made in developing high-performance cathodes,the Zn anode issues,such as Zn dendrites,corrosion,and hydrogen evolution,have been observed to shorten ZIB’s lifespan seriously,thus restricting their practical application.Engineering advanced Zn anodes based on two-dimensional(2D)materials are widely investigated to address these issues.With atomic thickness,2D materials possess ultrahigh specific surface area,much exposed active sites,superior mechanical strength and flexibility,and unique electrical properties,which confirm to be a promising alternative anode material for ZIBs.This review aims to boost rational design strategies of 2D materials for practical application of ZIB by combining the fundamental principle and research progress.Firstly,the fundamental principles of 2D materials against the drawbacks of Zn anode are introduced.Then,the designed strategies of several typical 2D materials for stable Zn anodes are comprehensively summarized.Finally,perspectives on the future development of advanced Zn anodes by taking advantage of these unique properties of 2D materials are proposed.