The interfacial engineering in solid-state lithium batteries(SSLBs)is attracting escalating attention due to the profoundly enhanced safety,energy density,and charging capabilities of future power storage technologies...The interfacial engineering in solid-state lithium batteries(SSLBs)is attracting escalating attention due to the profoundly enhanced safety,energy density,and charging capabilities of future power storage technologies.Nonetheless,polymer/ceramic interphase compatibility,serious agglomeration of ceramic particles,and discontinuous ionic conduction at the electrode/electrolyte interface seriously limit Li^(+)transport in SSLBs and block the application and large-scale manufacturing.Hence,garnet Li_(7)La_(3)Zr_(2)O_(12)(LLZO)nanoparticles are introduced into the polyacrylonitrile(PAN)nanofiber to fabricate a polymer-ceramic nanofiber-enhanced ultrathin SSE membrane(3D LLZO-PAN),harnessing nanofiber confinement to aggregate LLZO nanoparticles to build the continuous conduction pathway of Li^(+).In addition,a novel integrated electrospinning process is deliberately designed to construct tight physical contact between positive electrode/electrolyte interphases.Importantly,the synergistic effect of the PAN,polyethylene oxide(PEO),and lithium bis((trifluoromethyl)sulfonyl)azanide(LiTFSI)benefits a stable solid electrolyte interphase(SEI)layer,resulting in superior cycling performance,achieving a remarkable 1500 h cycling at 0.2 mA cm^(-2) in the Li|3D LLZO-PAN|Li battery.Consequently,the integrated polymer-ceramic nanofiber-enhanced SSEs simultaneously achieve the balance in ultrathin thickness(16μm),fast ion transport(2.9×10^(-4) S cm^(-1)),and superior excellent interface contact(15.6Ω).The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)|3D LLZO-PAN|Li batteries(2.7-4.3 V)can work over 200 cycles at 0.5 C.The pouch cells with practical LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)||Li configuration achieve an ultrahigh energy density of 345.8 Wh kg^(-1) and safety performance.This work provides new strategies for the manufacturing and utilization of high-energy-density SSLBs.展开更多
Frequent heat waves and cold spells pose threats to human survival.Herein,we develop a multifunctional all-nanofiber cloth with physiological signal monitoring and personal thermal management capabilities through faci...Frequent heat waves and cold spells pose threats to human survival.Herein,we develop a multifunctional all-nanofiber cloth with physiological signal monitoring and personal thermal management capabilities through facile fiber electrospinning and ink printing techniques.The double-sided fabric mat of a thick carbon nanotube network with high solar absorption on top of a thermo-plastic polyurethane nanofiber substrate with high solar reflectivity and mid-infrared emissivity offers a contrary thermal management effect of heating or cooling by opposite wearing mode.The integrated fabric strain and tempera-ture sensors for health status evaluation through monitoring physiological signals of respiration and body temperature.By wearing a T-shirt tailored by the developed electronic cloth,the wearer's skin temperature can be actively regulated with cooling by 5.4℃and warming by 3.0℃in hot and cold environ-ments compared to normal clothing,respectively.This platform can inspire further studies in wearable multifunctional permeable electronics.展开更多
Lithium-ion batteries(LIBs)have dominated the market for a long time.However,the scarcity of lithium resources has sparked concerns about future energy storage devices,leading many researchers to turn their attention ...Lithium-ion batteries(LIBs)have dominated the market for a long time.However,the scarcity of lithium resources has sparked concerns about future energy storage devices,leading many researchers to turn their attention to other energy storage devices,such as sodium-ion batteries(SIBs),potassiumion batteries(KIBs),zinc-ion batteries(ZIBs),and so on.Among them,SIBs have attracted widespread attention from researchers due to their abundant sodium resources,high safety,and excellent low-temperature performance.Because the cathode of the battery determines the energy density,cycle life,charge/discharge rate,and cost,the research on the cathodes for SIBs is particularly important.Layered oxide cathodes,with their periodic layered structure,good electrical conductivity,and two-dimensional ion transport channels,are regarded as the most promising cathode materials for SIBs.Currently,the main issues facing layered oxide cathodes include irreversible phase transitions,high air sensitivity,insufficient energy density,surface residual alkali,and the migration and dissolution of transition metals.The key to solving these problems lies in the development of a new generation of high-performance layered oxide cathodes.Hence,we review the current research progress of layered oxide cathode materials for SIBs and various optimizing strategies,and finally summarize and provide an outlook on the future development trends of SIBs.展开更多
Hydrogel-based sensors are recognized as key players in revolutionizing robotic applications,healthcare monitoring,and the development of artificial skins.However,the primary challenge hindering the commercial adoptio...Hydrogel-based sensors are recognized as key players in revolutionizing robotic applications,healthcare monitoring,and the development of artificial skins.However,the primary challenge hindering the commercial adoption of hydrogel-based sensors is their lack of high stability,which arises from the high water content within the hydrogel structure,leading to freezing at subzero temperatures and drying issues if the protective layer is compromised.These factors result in a significant decline in the benefits offered by aqueous gel electrolytes,particularly in terms of mechanical properties and conductivity,which are crucial for flexible wearable electronics.Previous reports have highlighted several disadvantages associated with using cryoprotectant co-solvents and lower mechanical properties for ion-doped anti-freezing hydrogel sensors.In this study,the design and optimization of a photocrosslinkable ionic hydrogel utilizing silk methacrylate as a novel natural crosslinker are presented.This innovative hydrogel demonstrates significantly enhanced mechanical properties,including stretchability(>1825%),tensile strength(2.49 MPa),toughness(9.85 MJ m^(-3)),and resilience(4%hysteresis),compared to its non-ion-doped counterpart.Additionally,this hydrogel exhibits exceptional nonfreezing behavior down to-85℃,anti-drying properties with functional stability up to 2.5 years,and a signal drift of only 5.35%over 2450 cycles,whereas the control variant,resembling commonly reported hydrogels,exhibits a signal drift of 149.8%.The successful application of the developed hydrogel in advanced robotics,combined with the pioneering demonstration of combinatorial commanding using a single sensor,could potentially revolutionize sensor design,elevating it to the next level and benefiting various fields.展开更多
Developing intelligent electromagnetic wave(EMW)absorption materials with real-time response-ability is of great significance in complex application environments.Herein,highly compressible Fe@CNFs@Co/C elastic aerogel...Developing intelligent electromagnetic wave(EMW)absorption materials with real-time response-ability is of great significance in complex application environments.Herein,highly compressible Fe@CNFs@Co/C elastic aerogels were assembled through the electrospinning method,achieving EMW absorption through pressure changes.By varying the pressure,the effective absorption bandwidth(EAB)of Fe@CNFs@Co/C elastic aerogels shows continuous changes from low frequency to high frequency.The EAB of Fe@CNFs@Co/C elastic aerogels is 14.4 GHz(3.36-17.76 GHz),which covers 90%of the range of S/C/X/Ku bands.The theoretical simulation indicates that the external pressure prompts a reduction in the spacing between the fiber layers in the aerogels and facilitates the formation of a 3D conductive network with enhanced attenuation ability of EMW.The uniform distribution of metal particles and appropriate layer spacing can effectively optimize the impedance matching to achieve the best EMW absorption performance.This work state clearly that the hierarchically assembled elastic aerogels composed of metal-organic frameworks(MOFs)derivatives and carbon fibers are ideal dynamic EMW absorption materials for intelligent EMW response.展开更多
Dual-band photodetectors exhibit considerable advantages in target discrimination and navigation compared to single-band devices in complex circumstances.However,it remains a major challenge to overcome the limitation...Dual-band photodetectors exhibit considerable advantages in target discrimination and navigation compared to single-band devices in complex circumstances.However,it remains a major challenge to overcome the limitations of traditional devices in terms of their integration with multiple light-absorbing layers and complicated optical components.In this study,a visible and nearinfrared(NIR)dual-band polarimetric photodetector with a single lightabsorbing layer is constructed by utilizing the distinctive conversion of linear dichroism(LD)polarity in two-dimensional niobium trisulfide(NbS_(3)).The NbS_(3)photodetector exhibits selective detection behaviors in the visible and NIR bands,in which by switching the polarization angle of the incident light from 0°to 90°,photocurrent decreases in the visible region,and increases in the NIR region.Specifically,the degrees of linear polarization of photocurrent are 0.59 at 450 nm and-0.47 at 1300 nm,respectively.The opposite photoresponse in the visible and NIR bands of the photodetector significantly enhances the dual-band information recognition.Therefore,clear visible and NIR dual-band polarimetric imaging is accurately realized based on the NbS_(3)photodetector taking advantage of its fast response speed of 28μs.Such anisotropic materials,with unique LD conversion features,can facilitate selective modulation between the visible and NIR spectral ranges and promote the development of next-generation multi-dimensional photodetection for various applications,including com/puter vision,surveillance,and biomedical imaging.展开更多
Substance discrimination beyond the shape feature is urgently desired for x-ray imaging for enhancing target identification.With two x-ray sources or stacked two detectors,the two-energy-channel x-ray detection can di...Substance discrimination beyond the shape feature is urgently desired for x-ray imaging for enhancing target identification.With two x-ray sources or stacked two detectors,the two-energy-channel x-ray detection can discriminate substance density by normalizing the target thickness.Nevertheless,the artifacts,high radiation dose and difficulty in image alignment due to two sources or two detectors impede their widespread application.In this work,we report a single direct x-ray detector with MAPbI_(3)/MAPbBr_(3)heterojunction for switchable soft x-ray(<20 keV)and hard x-ray(>20 keV)detection under one x-ray source.Systematic characterizations confirm soft and hard x-ray deposit their energy in MAPbI_(3)and MAPbBr_(3)layer,respectively,while working voltages can control the collection of generated charge carriers in each layer for selective soft/hard x-ray detection.The switching rate between soft and hard x-ray detection mode reaches 100 Hz.Moreover,the detector possesses a moderate performance with~50 nGy s^(-1)in limit-of-detection,~8000μC Gy^(-1)cm^(-2)in sensitivity and ~7 lp/mm in imaging resolution.By defining the attenuation coefficient ratio(μL/μH)as substance label,we effectively mitigate the influence of target thickness and successfully discriminate substances in the acquired x-ray images.展开更多
Lithium batteries are becoming increasingly vital thanks to electric vehicles and large-scale energy storage.Carbon materials have been applied in battery cathode,anode,electrolyte,and separator to enhance the electro...Lithium batteries are becoming increasingly vital thanks to electric vehicles and large-scale energy storage.Carbon materials have been applied in battery cathode,anode,electrolyte,and separator to enhance the electrochemical performance of rechargeable lithium batteries.Their functions cover lithium storage,electrochemical catalysis,electrode protection,charge conduction,and so on.To rationally implement carbon materials,their properties and interactions with other battery materials have been probed by theoretical models,namely density functional theory and molecular dynamics.This review summarizes the use of theoretical models to guide the employment of carbon materials in advanced lithium batteries,providing critical information difficult or impossible to obtain from experiments,including lithiophilicity,energy barriers,coordination structures,and species distribution at interfaces.Carbon materials under discussion include zero-dimensional fullerenes and capsules,one-dimensional nanotubes and nanoribbons,two-dimensional graphene,and three-dimensional graphite and amorphous carbon,as well as their derivatives.Their electronic conductivities are explored,followed by applications in cathode and anode performance.While the role of theoretical models is emphasized,experimental data are also touched upon to clarify background information and show the effectiveness of strategies.Evidently,carbon materials prove promising in achieving superior energy density,rate performance,and cycle life,especially when informed by theoretical endeavors.展开更多
Fiber-shaped batteries,distinguished by their unique one-dimensional archi-tecture,offer ultra-high flexibility,remarkable stretchability,and excellent knittability,rendering them highly appealing as energy storage so...Fiber-shaped batteries,distinguished by their unique one-dimensional archi-tecture,offer ultra-high flexibility,remarkable stretchability,and excellent knittability,rendering them highly appealing as energy storage solutions for smart wearable fabrics.Among various fiber-shaped battery systems,aqueous zinc batteries stand out as one of the most promising candidates owing to their high specific capacity,inherent safety,and cost-effectiveness.However,the practical applicability of fiber-shaped zinc batteries(FZBs)is significantly hin-dered by challenges in scalable production,long-term operational stability,and seamless integration.Despite the growing interest in FZBs,a comprehen-sive and systematic review that critically examines the essential components,assembly configurations,manufacturing techniques,and performance-enhancing strategies is still lacking.This review aims to fill this gap by first summarizing the fundamental components of FZBs,including cathodes,anodes,electrolytes,current collectors,and encapsulation materials.It then compares the impact of various assembly configurations,including parallel,winding,coaxial,and weaving structures,on battery performance.Further-more,it provides an in-depth analysis of diverse manufacturing techniques for fiber electrodes,including dip-coating,hydrothermal synthesis,and electrode-position,as well as the assembly procedures ranging from manual to equipment-assisted and one-step assembly methods.In addition,this review highlights strategies for improving both electrochemical and wearable perfor-mance through material modification and structural design.It also under-scores the multifunctional applications of FZBs,such as thermosensitive,fluorescent,and sweat-driven variants,along with their potential in physiologi-cal sensing and environmental monitoring.Finally,it identifies the existing barriers to FZBs commercialization,including limited energy density,complex integration processes,and unclear internal mechanisms.Based on these insights,it proposes future research directions and development initiatives to advance the field of FZBs,thereby promoting their transition from laboratory prototypes to commercial products.展开更多
Metal oxide-supported multielement alloy nanoparticles are very promising as highly efficient and cost-effective catalysts with a virtually unlimited compositional space.However,controllable synthesis of ultrasmall mu...Metal oxide-supported multielement alloy nanoparticles are very promising as highly efficient and cost-effective catalysts with a virtually unlimited compositional space.However,controllable synthesis of ultrasmall multielement alloy nanoparticles(us-MEA-NPs)supported on porous metal oxides with a homogeneous elemental distribution and good catalytic stability during long-term operation is extremely challenging due to their oxidation and strong immiscibility.As a proof of concept that such synthesis can be realized,this work presents a general“bottom-up”l ultrasonic-assisted,simultaneous electro-oxidation–reduction-precipitation strategy for alloying dissimilar elements into single NPs on a porous support.One characteristic of this technique is uniform mixing,which results from simultaneous rapid thermal decomposition and reduction and leads to multielement liquid droplet solidification without aggregation.This process was achieved through a synergistic combination of enhanced electrochemical and plasma-chemical phenomena at the metal–electrolyte interface(electron energy of 0.3–1.38 eV at a peak temperature of 3000 K reached within seconds at a rate of105 K per second)in an aqueous solution under an ultrasonic field(40 kHz).Illustrating the effectiveness of this approach,the CuAgNiFe-CoRuMn@MgO-P3000 catalyst exhibited exceptional catalytic efficiency in selective hydrogenation of nitro compounds,with over 99%chemoselectivity and nearly 100%conversion within 60 s and no decrease in catalytic activity even after 40 cycles(>98%conversion in 120 s).Our results provide an effective,transferable method for rationally designing supported MEA-NP catalysts at the atomic level and pave the way for a wide variety of catalytic reactions.展开更多
Triboelectric nanogenerators(TENGs)as a clean energy-harvesting technology are experiencing significant growth in the pursuit of carbon neutrality,accompanied by the increasing use of environmentally friendly biomater...Triboelectric nanogenerators(TENGs)as a clean energy-harvesting technology are experiencing significant growth in the pursuit of carbon neutrality,accompanied by the increasing use of environmentally friendly biomaterials.However,biomaterials exhibit inferior triboelectric properties compared with petromaterials,hindering the development of bio-based TENGs.Here,leveraging the crystal boundary-tuning strategy,we develop a chitosan aerogel-based TENG(CS-TENG)that is capable of delivering power density over 116 W m-2,beyond that of the previous reports for CS-TENG by an order of magnitude.With a high output voltage of 3200 V,the CS-TENG directly illuminated 1000 LEDs in series.Notably,the CS aerogel exhibits self-healing,waste recycling and gas-sensitive properties,ensuring the long-term durability,environmental benignity and sensing characteristics of the CS-TENG.Furthermore,a breathactivated mask-integrated CS-TENG ammonia monitoring system is engineered,which accurately detects changes in ammonia concentration within the range of 10-160 ppm,enabling real-time monitoring of ammonia in the environment.Our results set a record for the ultrahigh power density of CS-TENG,representing a significant advancement in the practical application of TENGs.展开更多
Muscles,the fundamental components supporting all human movement,exhibit various signals upon contraction,including mechanical signals indicat-ing tremors or mechanical deformation and electrical signals responsive to...Muscles,the fundamental components supporting all human movement,exhibit various signals upon contraction,including mechanical signals indicat-ing tremors or mechanical deformation and electrical signals responsive to muscle fiber activation.For noninvasive wearable devices,these signals can be measured using surface electromyography(sEMG)and force myography(FMG)techniques,respectively.However,relying on a single source of infor-mation is insufficient for a comprehensive evaluation of muscle condition.In order to accurately and effectively evaluate the various states of muscles,it is necessary to integrate sEMG and FMG in a spatiotemporally synchronized manner.This study presents a flexible sensor for multimodal muscle state monitoring,integrating serpentine-structured sEMG electrodes with fingerprint-like FMG sensors into a patch approximately 250μm thick.This design achieves a multimodal assessment of muscle conditions while maintaining a compact form factor.A thermo-responsive adhesive hydrogel is incorporated to enhance skin adhesion,improving the signal-to-noise ratio of the sEMG signals(33.07 dB)and ensuring the stability of the FMG sensor dur-ing mechanical deformation and tremors.The patterned coupled sensing patch demonstrates its utility in tracking muscular strength,assessing fatigue levels,and discerning features of muscle dysfunction by analyzing the time-domain and frequency-domain characteristics of the mechanical–electrical coupled signals,highlighting its potential application in sports training and rehabilita-tion monitoring.展开更多
Photoelectric memristors have shown great potential for future machine visions,via integrating sensing,memory,and computing(namely“all-in-one”)functions in a single device.However,their hard-to-tune photoresponse be...Photoelectric memristors have shown great potential for future machine visions,via integrating sensing,memory,and computing(namely“all-in-one”)functions in a single device.However,their hard-to-tune photoresponse behav-ior necessitates extra function modules for signal encoding and modality con-version,impeding such integration.Here,we report an all-in-one memristor with Cs_(2)AgBiBr_(6) perovskite,where the Br vacancy doping-endowed tunable energy band enables tunable photoresponsivity(TPR)behavior.As a result,the memristor showed a large tunable ratio of 35.9 dB,while its photoresponsivity presented a maximum of 2.7×10^(3)mA W^(-1)and a long-term memory behavior with over 10^(4)s,making it suitable for realizing all-in-one processing tasks.By mapping the algorithm parameters onto the photoresponsivity,we successfully performed both recognition and processing tasks based on the TPR memristor array.Remarkably,compared with conventional complementary metal–oxide–semiconductor counterparts,our demonstrations provided comparable perfor-mance but had-133-fold and-299-fold reductions in energy consumption,respectively.Our work could facilitate the development of all-in-one smart devices for next-generation machine visions.展开更多
Since its emergence in 2009,perovskite photovoltaic technology has achieved remarkable progress,with efficiencies soaring from 3.8%to over 26%.Despite these advancements,challenges such as long-term material and devic...Since its emergence in 2009,perovskite photovoltaic technology has achieved remarkable progress,with efficiencies soaring from 3.8%to over 26%.Despite these advancements,challenges such as long-term material and device stability remain.Addressing these challenges requires reproducible,user-independent laboratory processes and intelligent experimental preselection.Traditional trial-and-error methods and manual analysis are inefficient and urgently need advanced strategies.Automated acceleration platforms have transformed this field by improving efficiency,minimizing errors,and ensuring consistency.This review summarizes recent developments in machine learning-driven auto-mation for perovskite photovoltaics,with a focus on its application in new transport material discovery,composition screening,and device preparation optimization.Furthermore,the review introduces the concept of the self-driven Autonomous Material and Device Acceleration Platforms(AMADAP)labora-tory and discusses potential challenges it may face.This approach streamlines the entire process,from material discovery to device performance improve-ment,ultimately accelerating the development of emerging photovoltaic technologies.展开更多
Nickel-rich layered oxides(LiNixCoyMnzO2,NCM)are among the most promising cathode materials for high-energy lithium-ion batteries,offering high specific capacity and output voltage at a relatively low cost.However,ind...Nickel-rich layered oxides(LiNixCoyMnzO2,NCM)are among the most promising cathode materials for high-energy lithium-ion batteries,offering high specific capacity and output voltage at a relatively low cost.However,industrialscale co-precipitation presents significant challenges,particularly in maintaining particle sphericity,ensuring a stable concentration gradient,and preserving production yield when transitioning from lab-scale compositions.This study addresses a critical issue in the large-scale synthesis of nickel-rich NCM(x=0.8381):nickel leaching,which compromises particle uniformity and battery performance.To mitigate this,we optimize the reaction process and develop an artificial intelligence-driven defect prediction system that enhances precursor stability.Our domain adaptation based machine learning model,which accounts for equipment wear and environmental variations,achieves a defect detection accuracy of 97.8%based on machine data and process conditions.By implementing this approach,we successfully scale up NCM precursor production to over 2 tons,achieving 83%capacity retention after 500 cycles at a 1C rate.In addition,the proposed approach demonstrates the formation of a concentration gradient in the composition and a high sphericity of 0.951(±0.0796).This work provides new insights into the stable mass production of NCM precursors,ensuring both high yield and performance reliability.展开更多
The simultaneous enhancement of magnetic and dielectric properties in nanomaterials is becoming increasingly important for achieving exceptional microwave absorption performance.However,the engineering strategies for ...The simultaneous enhancement of magnetic and dielectric properties in nanomaterials is becoming increasingly important for achieving exceptional microwave absorption performance.However,the engineering strategies for modulating electromagnetic responses remain challenging,and the underlying magnetic-dielectric loss mechanisms are not yet fully understood.In this study,we constructed novel dual-coupling networks through the tightly packed Fe_(3)O_(4)@C spindles,which exhibit both dielectric and magnetic dissipation effects.During the spray-drying process,vigorous self-assembly facilitated the formation of hierarchical microspheres composed of nanoscale core-shell ferromagnetic units.Numerous heterogeneous interfaces and abundant magnetic domains were produced in these microspheres.The integrated dielectric/magnetic coupling networks,formed by discontinuous carbon layers and closely arranged Fe_(3)O_(4)spindles,contribute to strong absorption through intense interfacial polarization and magnetic interactions.The mechanisms behind both magnetic and dielectric losses are elucidated through Lorentz electron holography and micromagnetic simulations.Consequently,the hierarchical microspheres demonstrate excellent low-frequency absorption performance,achieving an effective absorption bandwidth of 3.52 GHz,covering the entire C-band from 4 to 8 GHz.This study reveals that dual-coupling networks engineering is an effective strategy for synergistically enhancing electromagnetic responses and improving the absorption performance of magnetic nanomaterials.展开更多
Defect engineering in photocatalytic materials has garnered significant interest due to the considerable impact of defects on light absorption,charge separation,and surface reaction dynamics.However,a limited understa...Defect engineering in photocatalytic materials has garnered significant interest due to the considerable impact of defects on light absorption,charge separation,and surface reaction dynamics.However,a limited understanding of how these defects influence photocatalytic properties remains a persistent challenge.This review comprehensively analyzes the vital role of defect engineering for enhancing the photocatalytic performance,highlighting its significant influence on material properties and efficiency.It systematically classifies defect types,including vacancy defects(oxygen and metal vacancies),doping defects(anion and cation),interstitial defects,surface defects(step edges,terraces,kinks,and disordered layers),antisite defects,and interfacial defects in the core–shell structures and heterostructure borders.The impact of complex defect groups and manifold defects on improved photocatalytic performance is also examined.The review emphasizes the principal benefits of defect engineering,including the enhancement of light adsorption,reduction of band gaps,improved charge separation and movements,and suppression of charge recombination.These enhancements lead to a boost in catalytic active sites,optimization of electronic structures,tailored band alignments,and the development of mid-gap states,leading to improved structural stability,photocorrosion resistance,and better reaction selectivity.Furthermore,the most recent improvements,such as oxygen vacancies,nitrogen and sulfur doping,surface defect engineering,and innovations in heterostructures,defect-rich metal–organic frameworks,and defective nanostructures,are examined comprehensively.This study offers essential insights into modern techniques and approaches in defect engineering,highlighting its significance in addressing challenges in photocatalytic materials and promoting the advancement of effective and adaptable platforms for renewable energy and environmental uses.展开更多
Thin-film composite(TFC)membranes featuring nanovoid-containing polyam-ide(PA)layers on supportive nanofiber substrates represent a significant advancement in desalination technology.However,the separation perfor-manc...Thin-film composite(TFC)membranes featuring nanovoid-containing polyam-ide(PA)layers on supportive nanofiber substrates represent a significant advancement in desalination technology.However,the separation perfor-mance of TFC membranes hinges critically on the nanoscale thickness of the PA layers and their distinctive ridge-and-valley roughness.This complex mor-phology is a direct result of interfacial instability arising during the highly exo-thermic interfacial polymerization(IP),where heat generation drives non-uniform PA layer growth.To mitigate these instabilities that adversely affect the overall membrane performance,thermally conductive MXene(Ti_(3)C_(2)T_(x))nanosheets are spray-coated onto the supportive polymeric substrates before initiating the IP process.The MXene-coated substrate significantly improves the surface morphology of the PA layer,reducing its thickness to 18 nm and minimizing nanovoid formation due to the effective lateral heat dissipation by the Ti_(3)C_(2)T_(x)MXene interlayer.These interlayers regulate monomer diffusion via hydrogen bonding and covalent interactions,ensuring uniform polymeriza-tion and defect-free PA layers.The optimized Ti_(3)C_(2)T_(x)MXene-interlayered TFC membrane exhibits a more than two-fold increase in the water flux,exceeding that of commercial membranes,while significantly improving ion rejection.This study highlights the significant impact of substrate thermal conductivity on desalination efficiency,enabling the development of smooth and efficient PA nanofilms for high-performance desalination through the tailored design of interlayered TFC membranes.展开更多
Ternary MAX phases,characterized by the chemical formula M₂AX,represent a group of layered materials with hexagonal lattices.These MAX phases have been the subject of extensive experimental and theoretical studies.For...Ternary MAX phases,characterized by the chemical formula M₂AX,represent a group of layered materials with hexagonal lattices.These MAX phases have been the subject of extensive experimental and theoretical studies.Formation energy and thermodynamic calculations indicate that MAX phases containing late transition metals,such as Rh,Ru,Pt,Pd,Co,and Ni,are unlikely to form.Here,we introduce an alternative family of orthorhombic and monoclinic materials,the LAX phases,which exhibit similarities to MAX phases in terms of their layered structure and A and X elements.However,LAX materials incorporate late transition metals in place of the early transition metals.Advanced techniques for predicting the crystal structure of materials,coupled with data-driven materials research and machine learning algorithms,were employed to investigate the stable structures containing transition metals from the last groups of the d-block elements.The analyses revealed 207 ternary LAX systems that demonstrate robust stability against decomposition,with 100 of these systems showing dynamic stability.An in-depth examination of the top 10 structures revealed five LAX systems that are phase stable and exhibit superior mechanical properties,outperforming MAX phase counterparts in Young's modulus,stiffness,and hardness.These findings indicate that many LAX phase structures are viable candidates for future synthesis,highlighting the potential of heuristic-based structure searches in material discovery.展开更多
Metallizing 2D semiconductors is a crucial research area with significant applications,such as reducing the contact resistance at metal/2D semiconductor interfaces.This is a key challenge in the realization of next-ge...Metallizing 2D semiconductors is a crucial research area with significant applications,such as reducing the contact resistance at metal/2D semiconductor interfaces.This is a key challenge in the realization of next-generation lowpower and high-performance devices.While various methods exist for metallizing Mo-and W-based 2D semiconductors like MoS_(2) and WSe_(2),effective approaches for Pt-based ones have been lacking.This study demonstrates that platinum dichalcogenides(PtX_(2),X=Se or Te)undergo a semiconductorto-metal transition when grown on niobium dichalcogenides(NbX_(2),X=Se or Te).PtX_(2)/NbX_(2) heterostructures were fabricated using molecular beam epitaxy(MBE)and characterized by Raman spectra,scanning transmission electron microscopy(STEM)and scanning tunneling microscopy/spectroscopy(STM/STS).Raman spectra and STEM confirm the growth of 1T-phase PtX_(2) and 1H-phase NbX_(2).Both 2D STS mapping and layer-dependent STS show that regardless of their layer numbers,both pristine semiconducting PtSe_(2) and PtTe_(2) are converted to metallic forms when interfacing with NbSe_(2) or NbTe_(2).Density functional theory(DFT)calculations suggest that the metallization of PtSe_(2) on NbX_(2) and PtTe_(2) on NbTe_(2) results from interfacial orbital hybridization,while for PtTe_(2) on NbSe_(2),it is due to the strong p-doping effect caused by interfacial charge transfer.Our work provides an effective method for metallizing PtX_(2) semiconductors,which may lead to significant applications such as reducing the contact resistance at metal electrode/2D semiconductor interfaces and developing devices like rectifiers,rectenna,and photodetectors based on 2D Schottky diodes.展开更多
基金the National Key R&D Program of China(2023YFB2503902)the National Natural Science Foundation of China(U21A2080 and 22479009)National related project are gratefully acknowledged.
文摘The interfacial engineering in solid-state lithium batteries(SSLBs)is attracting escalating attention due to the profoundly enhanced safety,energy density,and charging capabilities of future power storage technologies.Nonetheless,polymer/ceramic interphase compatibility,serious agglomeration of ceramic particles,and discontinuous ionic conduction at the electrode/electrolyte interface seriously limit Li^(+)transport in SSLBs and block the application and large-scale manufacturing.Hence,garnet Li_(7)La_(3)Zr_(2)O_(12)(LLZO)nanoparticles are introduced into the polyacrylonitrile(PAN)nanofiber to fabricate a polymer-ceramic nanofiber-enhanced ultrathin SSE membrane(3D LLZO-PAN),harnessing nanofiber confinement to aggregate LLZO nanoparticles to build the continuous conduction pathway of Li^(+).In addition,a novel integrated electrospinning process is deliberately designed to construct tight physical contact between positive electrode/electrolyte interphases.Importantly,the synergistic effect of the PAN,polyethylene oxide(PEO),and lithium bis((trifluoromethyl)sulfonyl)azanide(LiTFSI)benefits a stable solid electrolyte interphase(SEI)layer,resulting in superior cycling performance,achieving a remarkable 1500 h cycling at 0.2 mA cm^(-2) in the Li|3D LLZO-PAN|Li battery.Consequently,the integrated polymer-ceramic nanofiber-enhanced SSEs simultaneously achieve the balance in ultrathin thickness(16μm),fast ion transport(2.9×10^(-4) S cm^(-1)),and superior excellent interface contact(15.6Ω).The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)|3D LLZO-PAN|Li batteries(2.7-4.3 V)can work over 200 cycles at 0.5 C.The pouch cells with practical LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)||Li configuration achieve an ultrahigh energy density of 345.8 Wh kg^(-1) and safety performance.This work provides new strategies for the manufacturing and utilization of high-energy-density SSLBs.
基金supported by the Tianjin Science and Technology Plan Project(22JCZDJC00630)the China National Key Research and Development Program(2024YFE0100400,2022YFC3601400)+6 种基金the National Natural Science Foundation of China(62311540155,52302041)the Higher Education Institution Science and Technology Research Project of Hebei Province(JZX2024024),the Tianjin Municipal Education Commission Research Project(2022KJ094)the Natural Science Foundation of Shandong Province(ZR2020ME120)the Development Plan for the Youth Innovation Teams in Universities of Shandong Province(2023KJ109)the Jinan City University Integration Development Strategy Project(JNSX2023017)the Taishan Scholars Project Special Funds(tsqn202312035)the Open Research Foundation of State Key Laboratory of Integrated Chips and Systems.
文摘Frequent heat waves and cold spells pose threats to human survival.Herein,we develop a multifunctional all-nanofiber cloth with physiological signal monitoring and personal thermal management capabilities through facile fiber electrospinning and ink printing techniques.The double-sided fabric mat of a thick carbon nanotube network with high solar absorption on top of a thermo-plastic polyurethane nanofiber substrate with high solar reflectivity and mid-infrared emissivity offers a contrary thermal management effect of heating or cooling by opposite wearing mode.The integrated fabric strain and tempera-ture sensors for health status evaluation through monitoring physiological signals of respiration and body temperature.By wearing a T-shirt tailored by the developed electronic cloth,the wearer's skin temperature can be actively regulated with cooling by 5.4℃and warming by 3.0℃in hot and cold environ-ments compared to normal clothing,respectively.This platform can inspire further studies in wearable multifunctional permeable electronics.
基金National Key Research and Development Program of China,Grant/Award Number:2023YFB3809303National Natural Science Foundation of China,Grant/Award Number:U21A2033251771076+1 种基金Guangdong Basic and Applied Basic Research Foundation,Grant/Award Numbers:2020B1515120049,2021A1515010332,2021A1515010153Research and Development Program in Key Areas of Guangdong Province,Grant/Award Number:2020B0101030005。
文摘Lithium-ion batteries(LIBs)have dominated the market for a long time.However,the scarcity of lithium resources has sparked concerns about future energy storage devices,leading many researchers to turn their attention to other energy storage devices,such as sodium-ion batteries(SIBs),potassiumion batteries(KIBs),zinc-ion batteries(ZIBs),and so on.Among them,SIBs have attracted widespread attention from researchers due to their abundant sodium resources,high safety,and excellent low-temperature performance.Because the cathode of the battery determines the energy density,cycle life,charge/discharge rate,and cost,the research on the cathodes for SIBs is particularly important.Layered oxide cathodes,with their periodic layered structure,good electrical conductivity,and two-dimensional ion transport channels,are regarded as the most promising cathode materials for SIBs.Currently,the main issues facing layered oxide cathodes include irreversible phase transitions,high air sensitivity,insufficient energy density,surface residual alkali,and the migration and dissolution of transition metals.The key to solving these problems lies in the development of a new generation of high-performance layered oxide cathodes.Hence,we review the current research progress of layered oxide cathode materials for SIBs and various optimizing strategies,and finally summarize and provide an outlook on the future development trends of SIBs.
基金H2020 Marie Skłodowska-Curie Actions,Grant/Award Number:899987Villum Fonden,Grant/Award Number:VIL60794。
文摘Hydrogel-based sensors are recognized as key players in revolutionizing robotic applications,healthcare monitoring,and the development of artificial skins.However,the primary challenge hindering the commercial adoption of hydrogel-based sensors is their lack of high stability,which arises from the high water content within the hydrogel structure,leading to freezing at subzero temperatures and drying issues if the protective layer is compromised.These factors result in a significant decline in the benefits offered by aqueous gel electrolytes,particularly in terms of mechanical properties and conductivity,which are crucial for flexible wearable electronics.Previous reports have highlighted several disadvantages associated with using cryoprotectant co-solvents and lower mechanical properties for ion-doped anti-freezing hydrogel sensors.In this study,the design and optimization of a photocrosslinkable ionic hydrogel utilizing silk methacrylate as a novel natural crosslinker are presented.This innovative hydrogel demonstrates significantly enhanced mechanical properties,including stretchability(>1825%),tensile strength(2.49 MPa),toughness(9.85 MJ m^(-3)),and resilience(4%hysteresis),compared to its non-ion-doped counterpart.Additionally,this hydrogel exhibits exceptional nonfreezing behavior down to-85℃,anti-drying properties with functional stability up to 2.5 years,and a signal drift of only 5.35%over 2450 cycles,whereas the control variant,resembling commonly reported hydrogels,exhibits a signal drift of 149.8%.The successful application of the developed hydrogel in advanced robotics,combined with the pioneering demonstration of combinatorial commanding using a single sensor,could potentially revolutionize sensor design,elevating it to the next level and benefiting various fields.
基金supported by the National Natural Science Foundation of China(Grant No.51772177)the Key Research and Development Program of Shaanxi Province(Grant No.2022GY-347).
文摘Developing intelligent electromagnetic wave(EMW)absorption materials with real-time response-ability is of great significance in complex application environments.Herein,highly compressible Fe@CNFs@Co/C elastic aerogels were assembled through the electrospinning method,achieving EMW absorption through pressure changes.By varying the pressure,the effective absorption bandwidth(EAB)of Fe@CNFs@Co/C elastic aerogels shows continuous changes from low frequency to high frequency.The EAB of Fe@CNFs@Co/C elastic aerogels is 14.4 GHz(3.36-17.76 GHz),which covers 90%of the range of S/C/X/Ku bands.The theoretical simulation indicates that the external pressure prompts a reduction in the spacing between the fiber layers in the aerogels and facilitates the formation of a 3D conductive network with enhanced attenuation ability of EMW.The uniform distribution of metal particles and appropriate layer spacing can effectively optimize the impedance matching to achieve the best EMW absorption performance.This work state clearly that the hierarchically assembled elastic aerogels composed of metal-organic frameworks(MOFs)derivatives and carbon fibers are ideal dynamic EMW absorption materials for intelligent EMW response.
基金supported by the National Natural Science Foundation of China(NSFC)-Research Grant Council of Hong Kong(RGC)Key International(Regional)Joint Research Program(NSFC Grant No.62261160574)NSFC Grant No.51872337+2 种基金the Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2024A1515010295,2022A1515110707,and 2021A1515012592)the China Postdoctoral Science Foundation(CPSF)(Grant Nos.2024M752105 and 2024T170580)Postdoctoral Fellowship Program of CPSF(GZB20230450).
文摘Dual-band photodetectors exhibit considerable advantages in target discrimination and navigation compared to single-band devices in complex circumstances.However,it remains a major challenge to overcome the limitations of traditional devices in terms of their integration with multiple light-absorbing layers and complicated optical components.In this study,a visible and nearinfrared(NIR)dual-band polarimetric photodetector with a single lightabsorbing layer is constructed by utilizing the distinctive conversion of linear dichroism(LD)polarity in two-dimensional niobium trisulfide(NbS_(3)).The NbS_(3)photodetector exhibits selective detection behaviors in the visible and NIR bands,in which by switching the polarization angle of the incident light from 0°to 90°,photocurrent decreases in the visible region,and increases in the NIR region.Specifically,the degrees of linear polarization of photocurrent are 0.59 at 450 nm and-0.47 at 1300 nm,respectively.The opposite photoresponse in the visible and NIR bands of the photodetector significantly enhances the dual-band information recognition.Therefore,clear visible and NIR dual-band polarimetric imaging is accurately realized based on the NbS_(3)photodetector taking advantage of its fast response speed of 28μs.Such anisotropic materials,with unique LD conversion features,can facilitate selective modulation between the visible and NIR spectral ranges and promote the development of next-generation multi-dimensional photodetection for various applications,including com/puter vision,surveillance,and biomedical imaging.
基金National Key Research and Development Program of China,Grant/Award Number:2022YFE0139100NSFC,Grant/Award Numbers:T2322003,52172146,62175028+1 种基金International Cooperative Research Project of Jiangsu Province,Grant/Award Number:BZ2022008Fundamental Research Funds for the Central Universities,Grant/Award Number:2242024K40017。
文摘Substance discrimination beyond the shape feature is urgently desired for x-ray imaging for enhancing target identification.With two x-ray sources or stacked two detectors,the two-energy-channel x-ray detection can discriminate substance density by normalizing the target thickness.Nevertheless,the artifacts,high radiation dose and difficulty in image alignment due to two sources or two detectors impede their widespread application.In this work,we report a single direct x-ray detector with MAPbI_(3)/MAPbBr_(3)heterojunction for switchable soft x-ray(<20 keV)and hard x-ray(>20 keV)detection under one x-ray source.Systematic characterizations confirm soft and hard x-ray deposit their energy in MAPbI_(3)and MAPbBr_(3)layer,respectively,while working voltages can control the collection of generated charge carriers in each layer for selective soft/hard x-ray detection.The switching rate between soft and hard x-ray detection mode reaches 100 Hz.Moreover,the detector possesses a moderate performance with~50 nGy s^(-1)in limit-of-detection,~8000μC Gy^(-1)cm^(-2)in sensitivity and ~7 lp/mm in imaging resolution.By defining the attenuation coefficient ratio(μL/μH)as substance label,we effectively mitigate the influence of target thickness and successfully discriminate substances in the acquired x-ray images.
基金supported by Beijing Natural Science Foundation(L233004)the National Key Research and Development Program(2021YFB2500300)+2 种基金the National Natural Science Foundation of China(T2322015,22109086,52394170,52394171,22109011,22393900,and 22108151)Tsinghua-Jiangyin Innovation Special Fund(TJISF)(2022JYTH0101)the Tsinghua University Initiative Scientific Research Program.
文摘Lithium batteries are becoming increasingly vital thanks to electric vehicles and large-scale energy storage.Carbon materials have been applied in battery cathode,anode,electrolyte,and separator to enhance the electrochemical performance of rechargeable lithium batteries.Their functions cover lithium storage,electrochemical catalysis,electrode protection,charge conduction,and so on.To rationally implement carbon materials,their properties and interactions with other battery materials have been probed by theoretical models,namely density functional theory and molecular dynamics.This review summarizes the use of theoretical models to guide the employment of carbon materials in advanced lithium batteries,providing critical information difficult or impossible to obtain from experiments,including lithiophilicity,energy barriers,coordination structures,and species distribution at interfaces.Carbon materials under discussion include zero-dimensional fullerenes and capsules,one-dimensional nanotubes and nanoribbons,two-dimensional graphene,and three-dimensional graphite and amorphous carbon,as well as their derivatives.Their electronic conductivities are explored,followed by applications in cathode and anode performance.While the role of theoretical models is emphasized,experimental data are also touched upon to clarify background information and show the effectiveness of strategies.Evidently,carbon materials prove promising in achieving superior energy density,rate performance,and cycle life,especially when informed by theoretical endeavors.
基金National Natural Science Foundation of China,Grant/Award Number:51702362Hunan Provincial Natural Science Foundation,Grant/Award Numbers:2022JJ30663,2022JJ40551Independent Science Foundation of National University of Defense Technology。
文摘Fiber-shaped batteries,distinguished by their unique one-dimensional archi-tecture,offer ultra-high flexibility,remarkable stretchability,and excellent knittability,rendering them highly appealing as energy storage solutions for smart wearable fabrics.Among various fiber-shaped battery systems,aqueous zinc batteries stand out as one of the most promising candidates owing to their high specific capacity,inherent safety,and cost-effectiveness.However,the practical applicability of fiber-shaped zinc batteries(FZBs)is significantly hin-dered by challenges in scalable production,long-term operational stability,and seamless integration.Despite the growing interest in FZBs,a comprehen-sive and systematic review that critically examines the essential components,assembly configurations,manufacturing techniques,and performance-enhancing strategies is still lacking.This review aims to fill this gap by first summarizing the fundamental components of FZBs,including cathodes,anodes,electrolytes,current collectors,and encapsulation materials.It then compares the impact of various assembly configurations,including parallel,winding,coaxial,and weaving structures,on battery performance.Further-more,it provides an in-depth analysis of diverse manufacturing techniques for fiber electrodes,including dip-coating,hydrothermal synthesis,and electrode-position,as well as the assembly procedures ranging from manual to equipment-assisted and one-step assembly methods.In addition,this review highlights strategies for improving both electrochemical and wearable perfor-mance through material modification and structural design.It also under-scores the multifunctional applications of FZBs,such as thermosensitive,fluorescent,and sweat-driven variants,along with their potential in physiologi-cal sensing and environmental monitoring.Finally,it identifies the existing barriers to FZBs commercialization,including limited energy density,complex integration processes,and unclear internal mechanisms.Based on these insights,it proposes future research directions and development initiatives to advance the field of FZBs,thereby promoting their transition from laboratory prototypes to commercial products.
基金National Research Foundation(NRF)funded by Republic of Korea,Grant/Award Number:NRF-2022R1A2C1004392Ministry of Science and ICT。
文摘Metal oxide-supported multielement alloy nanoparticles are very promising as highly efficient and cost-effective catalysts with a virtually unlimited compositional space.However,controllable synthesis of ultrasmall multielement alloy nanoparticles(us-MEA-NPs)supported on porous metal oxides with a homogeneous elemental distribution and good catalytic stability during long-term operation is extremely challenging due to their oxidation and strong immiscibility.As a proof of concept that such synthesis can be realized,this work presents a general“bottom-up”l ultrasonic-assisted,simultaneous electro-oxidation–reduction-precipitation strategy for alloying dissimilar elements into single NPs on a porous support.One characteristic of this technique is uniform mixing,which results from simultaneous rapid thermal decomposition and reduction and leads to multielement liquid droplet solidification without aggregation.This process was achieved through a synergistic combination of enhanced electrochemical and plasma-chemical phenomena at the metal–electrolyte interface(electron energy of 0.3–1.38 eV at a peak temperature of 3000 K reached within seconds at a rate of105 K per second)in an aqueous solution under an ultrasonic field(40 kHz).Illustrating the effectiveness of this approach,the CuAgNiFe-CoRuMn@MgO-P3000 catalyst exhibited exceptional catalytic efficiency in selective hydrogenation of nitro compounds,with over 99%chemoselectivity and nearly 100%conversion within 60 s and no decrease in catalytic activity even after 40 cycles(>98%conversion in 120 s).Our results provide an effective,transferable method for rationally designing supported MEA-NP catalysts at the atomic level and pave the way for a wide variety of catalytic reactions.
基金Key Program of the National Natural Science Foundation of China,Grant/Award Number:U22B2089General Program of National Natural Science Foundation of China,Grant/Award Number:52075061Science Fund for Distinguished Young Scholars of Chongqing,Grant/Award Number:CSTB2022 NSCQJQX0006。
文摘Triboelectric nanogenerators(TENGs)as a clean energy-harvesting technology are experiencing significant growth in the pursuit of carbon neutrality,accompanied by the increasing use of environmentally friendly biomaterials.However,biomaterials exhibit inferior triboelectric properties compared with petromaterials,hindering the development of bio-based TENGs.Here,leveraging the crystal boundary-tuning strategy,we develop a chitosan aerogel-based TENG(CS-TENG)that is capable of delivering power density over 116 W m-2,beyond that of the previous reports for CS-TENG by an order of magnitude.With a high output voltage of 3200 V,the CS-TENG directly illuminated 1000 LEDs in series.Notably,the CS aerogel exhibits self-healing,waste recycling and gas-sensitive properties,ensuring the long-term durability,environmental benignity and sensing characteristics of the CS-TENG.Furthermore,a breathactivated mask-integrated CS-TENG ammonia monitoring system is engineered,which accurately detects changes in ammonia concentration within the range of 10-160 ppm,enabling real-time monitoring of ammonia in the environment.Our results set a record for the ultrahigh power density of CS-TENG,representing a significant advancement in the practical application of TENGs.
基金National Key Research and Development Program of China,Grant/Award Number:2022YFE0111700National Natural Science Foundation of China,Grant/Award Numbers:T2125003,82202075+3 种基金Beijing Natural Science Foundation,Grant/Award Number:L212010National Postdoctoral Program for Innovative Talents,Grant/Award Number:BX20220380China Postdoctoral Science Foundation,Grant/Award Number:2022M710389Fundamental Research Funds for the Central Universities。
文摘Muscles,the fundamental components supporting all human movement,exhibit various signals upon contraction,including mechanical signals indicat-ing tremors or mechanical deformation and electrical signals responsive to muscle fiber activation.For noninvasive wearable devices,these signals can be measured using surface electromyography(sEMG)and force myography(FMG)techniques,respectively.However,relying on a single source of infor-mation is insufficient for a comprehensive evaluation of muscle condition.In order to accurately and effectively evaluate the various states of muscles,it is necessary to integrate sEMG and FMG in a spatiotemporally synchronized manner.This study presents a flexible sensor for multimodal muscle state monitoring,integrating serpentine-structured sEMG electrodes with fingerprint-like FMG sensors into a patch approximately 250μm thick.This design achieves a multimodal assessment of muscle conditions while maintaining a compact form factor.A thermo-responsive adhesive hydrogel is incorporated to enhance skin adhesion,improving the signal-to-noise ratio of the sEMG signals(33.07 dB)and ensuring the stability of the FMG sensor dur-ing mechanical deformation and tremors.The patterned coupled sensing patch demonstrates its utility in tracking muscular strength,assessing fatigue levels,and discerning features of muscle dysfunction by analyzing the time-domain and frequency-domain characteristics of the mechanical–electrical coupled signals,highlighting its potential application in sports training and rehabilita-tion monitoring.
基金National Key R&D Program,Grant/Award Numbers:2022YFB3204100,2021YFC3002200,2020YFA0709800National Natural Science Foundation of China,Grant/Award Numbers:U20A20168,51861145202,62374099,62304119+7 种基金STI 2030—Major Projects,Grant/Award Number:2022ZD0209200Tsinghua-Toyota Joint Research FundBeijing Natural Science Foundation-Xiaomi Innovation Joint Fund,Grant/Award Number:L233009China Postdoctoral Science Foundation,Grant/Award Numbers:2023M731882,BX20230188Independent Research Program of School of Integrated Circuits,Tsinghua UniversityGuoqiang Institute,Tsinghua UniversityFundamental Research Project of National Institute of Metrology China,Grant/Award Number:AKYCX2201Shuimu Tsinghua Scholar Program。
文摘Photoelectric memristors have shown great potential for future machine visions,via integrating sensing,memory,and computing(namely“all-in-one”)functions in a single device.However,their hard-to-tune photoresponse behav-ior necessitates extra function modules for signal encoding and modality con-version,impeding such integration.Here,we report an all-in-one memristor with Cs_(2)AgBiBr_(6) perovskite,where the Br vacancy doping-endowed tunable energy band enables tunable photoresponsivity(TPR)behavior.As a result,the memristor showed a large tunable ratio of 35.9 dB,while its photoresponsivity presented a maximum of 2.7×10^(3)mA W^(-1)and a long-term memory behavior with over 10^(4)s,making it suitable for realizing all-in-one processing tasks.By mapping the algorithm parameters onto the photoresponsivity,we successfully performed both recognition and processing tasks based on the TPR memristor array.Remarkably,compared with conventional complementary metal–oxide–semiconductor counterparts,our demonstrations provided comparable perfor-mance but had-133-fold and-299-fold reductions in energy consumption,respectively.Our work could facilitate the development of all-in-one smart devices for next-generation machine visions.
基金support of“ELF-PV-Design and development of solution processed functional materials for the next generations of PV technologies”(No.44-6521a/20/4)and“Solar Factory of the Future”(FKZ 20.2-3410.5-4-5)by the Bavarian State Governmentthe German Federal Ministry for Economic Affairs and Climate Action(project Pero4PV,FKZ:03EE1092A)+3 种基金SolMAP and SolarTAP-a Technology Acceleration Platform for emerging Photovoltaics project by Helmholtz Associationsupport from the China Scholarship Council(CSC)support from the Sino-German Postdoc Scholarship Program(CSC-DAAD)support from the Villum Foundation,Grant no.50440.Open Access funding enabled and organized by Projekt DEAL.
文摘Since its emergence in 2009,perovskite photovoltaic technology has achieved remarkable progress,with efficiencies soaring from 3.8%to over 26%.Despite these advancements,challenges such as long-term material and device stability remain.Addressing these challenges requires reproducible,user-independent laboratory processes and intelligent experimental preselection.Traditional trial-and-error methods and manual analysis are inefficient and urgently need advanced strategies.Automated acceleration platforms have transformed this field by improving efficiency,minimizing errors,and ensuring consistency.This review summarizes recent developments in machine learning-driven auto-mation for perovskite photovoltaics,with a focus on its application in new transport material discovery,composition screening,and device preparation optimization.Furthermore,the review introduces the concept of the self-driven Autonomous Material and Device Acceleration Platforms(AMADAP)labora-tory and discusses potential challenges it may face.This approach streamlines the entire process,from material discovery to device performance improve-ment,ultimately accelerating the development of emerging photovoltaic technologies.
基金Ministry of SMEs and Startups,Grant/Award Number:S3248116National Research Foundation of Korea,Grant/Award Numbers:RS-2023-00211636,RS-2024-00416891Ministry of Science and ICT,South Korea,Grant/Award Number:RS-2020-II201336。
文摘Nickel-rich layered oxides(LiNixCoyMnzO2,NCM)are among the most promising cathode materials for high-energy lithium-ion batteries,offering high specific capacity and output voltage at a relatively low cost.However,industrialscale co-precipitation presents significant challenges,particularly in maintaining particle sphericity,ensuring a stable concentration gradient,and preserving production yield when transitioning from lab-scale compositions.This study addresses a critical issue in the large-scale synthesis of nickel-rich NCM(x=0.8381):nickel leaching,which compromises particle uniformity and battery performance.To mitigate this,we optimize the reaction process and develop an artificial intelligence-driven defect prediction system that enhances precursor stability.Our domain adaptation based machine learning model,which accounts for equipment wear and environmental variations,achieves a defect detection accuracy of 97.8%based on machine data and process conditions.By implementing this approach,we successfully scale up NCM precursor production to over 2 tons,achieving 83%capacity retention after 500 cycles at a 1C rate.In addition,the proposed approach demonstrates the formation of a concentration gradient in the composition and a high sphericity of 0.951(±0.0796).This work provides new insights into the stable mass production of NCM precursors,ensuring both high yield and performance reliability.
基金National Natural Science Foundation of China,Grant/Award Numbers:52231007,12327804,T2321003,22088101National Key Research Program of China,Grant/Award Number:2021YFA1200600。
文摘The simultaneous enhancement of magnetic and dielectric properties in nanomaterials is becoming increasingly important for achieving exceptional microwave absorption performance.However,the engineering strategies for modulating electromagnetic responses remain challenging,and the underlying magnetic-dielectric loss mechanisms are not yet fully understood.In this study,we constructed novel dual-coupling networks through the tightly packed Fe_(3)O_(4)@C spindles,which exhibit both dielectric and magnetic dissipation effects.During the spray-drying process,vigorous self-assembly facilitated the formation of hierarchical microspheres composed of nanoscale core-shell ferromagnetic units.Numerous heterogeneous interfaces and abundant magnetic domains were produced in these microspheres.The integrated dielectric/magnetic coupling networks,formed by discontinuous carbon layers and closely arranged Fe_(3)O_(4)spindles,contribute to strong absorption through intense interfacial polarization and magnetic interactions.The mechanisms behind both magnetic and dielectric losses are elucidated through Lorentz electron holography and micromagnetic simulations.Consequently,the hierarchical microspheres demonstrate excellent low-frequency absorption performance,achieving an effective absorption bandwidth of 3.52 GHz,covering the entire C-band from 4 to 8 GHz.This study reveals that dual-coupling networks engineering is an effective strategy for synergistically enhancing electromagnetic responses and improving the absorption performance of magnetic nanomaterials.
基金Deanship of Research and Graduate Studies at King Khalid University,Grant/Award Number:RGP2/363/46。
文摘Defect engineering in photocatalytic materials has garnered significant interest due to the considerable impact of defects on light absorption,charge separation,and surface reaction dynamics.However,a limited understanding of how these defects influence photocatalytic properties remains a persistent challenge.This review comprehensively analyzes the vital role of defect engineering for enhancing the photocatalytic performance,highlighting its significant influence on material properties and efficiency.It systematically classifies defect types,including vacancy defects(oxygen and metal vacancies),doping defects(anion and cation),interstitial defects,surface defects(step edges,terraces,kinks,and disordered layers),antisite defects,and interfacial defects in the core–shell structures and heterostructure borders.The impact of complex defect groups and manifold defects on improved photocatalytic performance is also examined.The review emphasizes the principal benefits of defect engineering,including the enhancement of light adsorption,reduction of band gaps,improved charge separation and movements,and suppression of charge recombination.These enhancements lead to a boost in catalytic active sites,optimization of electronic structures,tailored band alignments,and the development of mid-gap states,leading to improved structural stability,photocorrosion resistance,and better reaction selectivity.Furthermore,the most recent improvements,such as oxygen vacancies,nitrogen and sulfur doping,surface defect engineering,and innovations in heterostructures,defect-rich metal–organic frameworks,and defective nanostructures,are examined comprehensively.This study offers essential insights into modern techniques and approaches in defect engineering,highlighting its significance in addressing challenges in photocatalytic materials and promoting the advancement of effective and adaptable platforms for renewable energy and environmental uses.
基金King Abdullah University of Science and Technology(KAUST),Saudi Arabia。
文摘Thin-film composite(TFC)membranes featuring nanovoid-containing polyam-ide(PA)layers on supportive nanofiber substrates represent a significant advancement in desalination technology.However,the separation perfor-mance of TFC membranes hinges critically on the nanoscale thickness of the PA layers and their distinctive ridge-and-valley roughness.This complex mor-phology is a direct result of interfacial instability arising during the highly exo-thermic interfacial polymerization(IP),where heat generation drives non-uniform PA layer growth.To mitigate these instabilities that adversely affect the overall membrane performance,thermally conductive MXene(Ti_(3)C_(2)T_(x))nanosheets are spray-coated onto the supportive polymeric substrates before initiating the IP process.The MXene-coated substrate significantly improves the surface morphology of the PA layer,reducing its thickness to 18 nm and minimizing nanovoid formation due to the effective lateral heat dissipation by the Ti_(3)C_(2)T_(x)MXene interlayer.These interlayers regulate monomer diffusion via hydrogen bonding and covalent interactions,ensuring uniform polymeriza-tion and defect-free PA layers.The optimized Ti_(3)C_(2)T_(x)MXene-interlayered TFC membrane exhibits a more than two-fold increase in the water flux,exceeding that of commercial membranes,while significantly improving ion rejection.This study highlights the significant impact of substrate thermal conductivity on desalination efficiency,enabling the development of smooth and efficient PA nanofilms for high-performance desalination through the tailored design of interlayered TFC membranes.
基金Iran National Science Foundation,Grant/Award Number:4025794Japan Society for the Promotion of Science,Grant/Award Number:24K08211。
文摘Ternary MAX phases,characterized by the chemical formula M₂AX,represent a group of layered materials with hexagonal lattices.These MAX phases have been the subject of extensive experimental and theoretical studies.Formation energy and thermodynamic calculations indicate that MAX phases containing late transition metals,such as Rh,Ru,Pt,Pd,Co,and Ni,are unlikely to form.Here,we introduce an alternative family of orthorhombic and monoclinic materials,the LAX phases,which exhibit similarities to MAX phases in terms of their layered structure and A and X elements.However,LAX materials incorporate late transition metals in place of the early transition metals.Advanced techniques for predicting the crystal structure of materials,coupled with data-driven materials research and machine learning algorithms,were employed to investigate the stable structures containing transition metals from the last groups of the d-block elements.The analyses revealed 207 ternary LAX systems that demonstrate robust stability against decomposition,with 100 of these systems showing dynamic stability.An in-depth examination of the top 10 structures revealed five LAX systems that are phase stable and exhibit superior mechanical properties,outperforming MAX phase counterparts in Young's modulus,stiffness,and hardness.These findings indicate that many LAX phase structures are viable candidates for future synthesis,highlighting the potential of heuristic-based structure searches in material discovery.
基金Ministry of Education Singapore,Grant/Award Number:MOET2EP50122-0020。
文摘Metallizing 2D semiconductors is a crucial research area with significant applications,such as reducing the contact resistance at metal/2D semiconductor interfaces.This is a key challenge in the realization of next-generation lowpower and high-performance devices.While various methods exist for metallizing Mo-and W-based 2D semiconductors like MoS_(2) and WSe_(2),effective approaches for Pt-based ones have been lacking.This study demonstrates that platinum dichalcogenides(PtX_(2),X=Se or Te)undergo a semiconductorto-metal transition when grown on niobium dichalcogenides(NbX_(2),X=Se or Te).PtX_(2)/NbX_(2) heterostructures were fabricated using molecular beam epitaxy(MBE)and characterized by Raman spectra,scanning transmission electron microscopy(STEM)and scanning tunneling microscopy/spectroscopy(STM/STS).Raman spectra and STEM confirm the growth of 1T-phase PtX_(2) and 1H-phase NbX_(2).Both 2D STS mapping and layer-dependent STS show that regardless of their layer numbers,both pristine semiconducting PtSe_(2) and PtTe_(2) are converted to metallic forms when interfacing with NbSe_(2) or NbTe_(2).Density functional theory(DFT)calculations suggest that the metallization of PtSe_(2) on NbX_(2) and PtTe_(2) on NbTe_(2) results from interfacial orbital hybridization,while for PtTe_(2) on NbSe_(2),it is due to the strong p-doping effect caused by interfacial charge transfer.Our work provides an effective method for metallizing PtX_(2) semiconductors,which may lead to significant applications such as reducing the contact resistance at metal electrode/2D semiconductor interfaces and developing devices like rectifiers,rectenna,and photodetectors based on 2D Schottky diodes.