Invasive as well as non-invasive neurotechnologies conceptualized to interface the central and peripheral nervous system have been probed for the past decades,which refer to electroencephalography,electrocorticography...Invasive as well as non-invasive neurotechnologies conceptualized to interface the central and peripheral nervous system have been probed for the past decades,which refer to electroencephalography,electrocorticography and microelectrode arrays.The challenges of these mentioned approaches are characterized by the bandwidth of the spatiotemporal resolution,which in turn is essential for large-area neuron recordings(Abiri et al.,2019).展开更多
High-performance alloys are indispensable in modern engineering because of their exceptional strength,ductility,corrosion resistance,fatigue resistance,and thermal stability,which are all significantly influenced by t...High-performance alloys are indispensable in modern engineering because of their exceptional strength,ductility,corrosion resistance,fatigue resistance,and thermal stability,which are all significantly influenced by the alloy interface structures.Despite substantial efforts,a comprehensive overview of interface engineering of high-performance alloys has not been presented so far.In this study,the interfaces in high-performance alloys,particularly grain and phase boundaries,were systematically examined,with emphasis on their crystallographic characteristics and chemical element segregations.The effects of the interfaces on the electrical conductivity,mechanical strength,toughness,hydrogen embrittlement resistance,and thermal stability of the alloys were elucidated.Moreover,correlations among various types of interfaces and advanced experimental and computational techniques were examined using big data analytics,enabling robust design strategies.Challenges currently faced in the field of interface engineering and emerging opportunities in the field are also discussed.The study results would guide the development of next-generation high-performance alloys.展开更多
A new method was proposed for preparing AZ31/1060 composite plates with a corrugated interface,which involved cold-pressing a corrugated surface on the Al plate and then hot-pressing the assembled Mg/Al plate.The resu...A new method was proposed for preparing AZ31/1060 composite plates with a corrugated interface,which involved cold-pressing a corrugated surface on the Al plate and then hot-pressing the assembled Mg/Al plate.The results show that cold-pressing produces intense plastic deformation near the corrugated surface of the Al plate,which promotes dynamic recrystallization of the Al substrate near the interface during the subsequent hot-pressing.In addition,the initial corrugation on the surface of the Al plate also changes the local stress state near the interface during hot pressing,which has a large effect on the texture components of the substrates near the corrugated interface.The construction of the corrugated interface can greatly enhance the shear strength by 2−4 times due to the increased contact area and the strong“mechanical gearing”effect.Moreover,the mechanical properties are largely depended on the orientation relationship between corrugated direction and loading direction.展开更多
Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving...Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.展开更多
Some active metal oxides(Al_(2)O_(3),TiO_(2),and Cr_(2)O_(3))were selected as dopants to the Al_(2)O_(3)-based ceramic shells for investment casting of K417G superalloy.The effects of dopant types and contents(0,2,5,a...Some active metal oxides(Al_(2)O_(3),TiO_(2),and Cr_(2)O_(3))were selected as dopants to the Al_(2)O_(3)-based ceramic shells for investment casting of K417G superalloy.The effects of dopant types and contents(0,2,5,and 8 wt.%)on the wettability and interfacial reaction between the alloy and shell were investigated by a sessile-drop experiment.The results show that increasing the Al_(2)O_(3) doping contents(0−8 wt.%)reduces the porosity(21.74%−10.08%)and roughness(3.22−1.34μm)of the shell surface.The increase in Cr_(2)O_(3) dopant content(2−8 wt.%)further exacerbates the interfacial reaction,leading to an increase in the thickness of the reaction layer(2.6−3.1μm)and a decrease in the wetting angle(93.9°−91.0°).The addition of Al_(2)O_(3) and TiO_(2) dopants leads to the formation of Al_(2)TiO_(5) composite oxides in the reaction products,which effectively inhibits the interfacial reaction.The increase in TiO_(2) dopant contents(0−8 wt.%)further promotes the formation of Al_(2)TiO_(5),which decreases the thickness of the interfacial reaction layer(3.9−1.2μm)and increases the wetting angle(95.0°−103.8°).The introduced dopants enhance the packing density of the shell surface,while simultaneously suppress the diffusion of active metal elements from the alloy matrix to the interface.展开更多
The O3-type NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(NFM)has emerged as a highly promising cathode material for sodiumion batteries due to its facile synthesis and high theoretical capacity.However,it suffers from severe capac...The O3-type NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(NFM)has emerged as a highly promising cathode material for sodiumion batteries due to its facile synthesis and high theoretical capacity.However,it suffers from severe capacity and rate capability degradation caused by multiple coupled failure mechanisms,including irreversible phase transitions,structural deterioration at high voltages,and electrolyte-induced surface corrosion.This work addresses the challenge of high-voltage stability in NFM cathodes via a synergistic bulk-phase and interface engineering strategy.Firstly,Li,Ti,and Co are codoped into the bulk lattice structure to suppress the Mn^(3+)-induced Jahn-Teller distortion and improve Na^(+)diffusion kinetics.And then,an AlPO_(4) protective coating layer is fabricated to mitigate electrolyte corrosion and interfacial side reactions.Consequently,the as-designed composite cathode(AP@NFMLTC)can effectively suppress the P3 to O3’phase transition within the voltage range of 2.0 to 4.2 V,resulting in a highly reversible sodium storage mechanism.After 100 cycles at a rate of 1 C,the capacity retention rate significantly improves from 45.6%to 83.6%,with a minimal voltage decay of just 0.08 V.The dual bulk-interface synergistic strategy in this work provides valuable insights into achieving high stable operation for sodium-ion batteries(SIBs)cathodes under enhanced voltage.展开更多
Practical application of Na_(3)SbS_(4)(NSS)solid-state electrolyte in sodium metal batteries has been significantly hindered by poor interfacial stability and insufficient ionic conductivity.In this study,a series of ...Practical application of Na_(3)SbS_(4)(NSS)solid-state electrolyte in sodium metal batteries has been significantly hindered by poor interfacial stability and insufficient ionic conductivity.In this study,a series of dual-site doped Na_(3-2x)Sb_(1-x)W_(x)S_(4-x)F_(x)(x=0,0.12,0.24,0.36)electrolytes through high-energy ball milling followed by high-temperature sintering is prepared,where tungsten(W)substitutes for antimony(Sb)and fluorine(F)replaces sulfur(S)in the NSS lattice.The co-doping of W and F not only broadens the interplanar spacing of NSS but also promotes the stable formation of the cubic phase of NSS,thereby effectively enhancing the transport ability of sodium ions within NSS.Among them,Na_(2.52)Sb_(0.76)W_(0.24)S_(3.76)F_(0.24) exhibits the highest ionic conductivity of 4.45 mS·cm^(-1).Furthermore,F doping facilitates the in-situ formation of NaF between the electrolyte and metallic sodium,significantly improving interfacial stability.Electrochemical evaluation shows that the Na/Na_(2.52)Sb_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na symmetric cell achieves a high critical current density of 1.65 mA·cm^(-2) and maintains stable sodium plating/stripping cycling for 500 h at 0.1 mA·cm^(-2).Additionally,the TiS2/Na_(2.52)Sb_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na full cell exhibits outstanding cycling stability and rate capability.展开更多
Metal-ceramic composites combine the excellent properties of metals and ceramics,which have high strength,stability,and corrosion re-sistance.Al_(2)O_(3)/FeCo composites have been proven to be useful in ap-plications ...Metal-ceramic composites combine the excellent properties of metals and ceramics,which have high strength,stability,and corrosion re-sistance.Al_(2)O_(3)/FeCo composites have been proven to be useful in ap-plications such as catalysts,mi-crowave absorption materials,and enhanced permeability dielectric.The understanding of the mechani-cal properties and dynamics at the atomic scale of the Al_(2)O_(3)/FeCo in-terface can promote the design and exploitment of metal-ceramic composites.In this work,we have obtained Young’s modulus and diffusion coefficient of the Al_(2)O_(3)/FeCo interface using molecular dynamics simulation,elucidated the structural characteristics of the Al_(2)O_(3)/FeCo interface at the atomic scale,and investigated the impact of atomic magnetism and the exter-nal magnetic field on the interface.Simulated results show that Young’s modulus of the Al_(2)O_(3)/FeCo interface is significantly improved compared with pure Al_(2)O_(3)and FeCo alloy at room and high temperatures.When the atomic magnetism and the external magnetic field are applied,Young’s modulus of the Al_(2)O_(3)/FeCo interface further increases to 612 GPa at 300 K and 602 GPa at 500 K.Moreover,the average density,diffusion coefficient,and radial distri-bution function are found to be modified substantially.This study will shed light on the atom-istic investigations of the metal-ceramic composites.展开更多
CsPbBr_(3)perovskite solar cells(PSCs)have attracted significant interest for their remarkable stability under high temperatures and humidity.However,challenges such as energy loss at the CsPbBr_(3)/oxide buried inter...CsPbBr_(3)perovskite solar cells(PSCs)have attracted significant interest for their remarkable stability under high temperatures and humidity.However,challenges such as energy loss at the CsPbBr_(3)/oxide buried interface and imperfect band alignment have impeded further efficiency enhancements.In this study,TiO_(2),SnO_(2),or ZnO was employed as electron transport layer(ETL)materials,respectively,in CsPbBr_(3)-based PSCs to optimize the band alignment at the ETL/CsPbBr_(3)interface and enhance the film quality of CsPbBr_(3)materials.The research findings indicate that the power conversion efficiency(PCE)of PSCs is influenced by the choice of ETL material.Specifically,TiO_(2)-based PSCs achieved a PCE of 10.37%efficiency,higher than SnO_(2)-or ZnO-based PSCs.This disparity in PCE can be attributed to variations in open-circuit voltage,which stem from different band alignments at the ETL/CsPbBr_(3)interface.Notably,superior photovoltaic performance was consistently observed in TiO_(2)-based PSCs due to the substantial conduction band offset(∆Ec)at the TiO_(2)/CsPbBr_(3)interface and the high quality of the CsPbBr_(3)film.This not only enhances electron extraction at the TiO_(2)/CsPbBr_(3)interface but also diminishes non-radiative recombination at the interface,as confirmed by density functional theory(DFT)calculations and experiments.Furthermore,photodetectors(PDs)based on TiO_(2)/CsPbBr_(3)heterojunction exhibit high photoresponse and photodetectivity.In conclusion,this study underscores the critical importance of the buried interface contact in CsPbBr_(3)and offers a direct approach for fabricating efficient and stable inorganic PSCs and PDs.展开更多
The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process o...The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process of 2D/3D heterojunction PSC on the stability of PSCs.Moreover,the evolution of the interface and carrier dynamic behavior of the 2D/3D perovskite films with long-term operation has not been systematically developed befo re.In this work,the effects of 2D/3 D heterojunction evolution on the interface of perovskite films and different carrier dynamics during 2D/3D evolution are systematically analyzed for the first time.The decomposition of 2D/3D heterojunction in the perovskite film will have a certain impact on the surface and carrier dynamics behavior of perovskite.During the evolution of 2D/3D heterojunction,PbI_(2)crystals will appear,which will improve the interfacial energy level matching between the electron transport layer and perovskite film.With a long evolution time,some holes will appear on the surface of perovskite film.The open circuit voltage(V_(OC))of PSCs increased from 1.14 to1.18 V and the PCE increased to 23.21%after 300 h storage in the nitrogen atmosphere,and maintained 89%initial performance for with 3000 h stability test in N_(2)box.This discovery has a significant role in promoting the development of inverted heterojunction PSCs and constructing the revolution mechanism of charge carrier dynamic.展开更多
Poly(3-hexylthiophene)(P3HT)is one of the most promising hole-transporting materials in the pursuit of efficient and stable perovskite solar cells due to its outstanding stability and low cost.However,the intrinsic lo...Poly(3-hexylthiophene)(P3HT)is one of the most promising hole-transporting materials in the pursuit of efficient and stable perovskite solar cells due to its outstanding stability and low cost.However,the intrinsic low carrier density of P3 HT and poor contact between the P3HT/perovskite interface always lead to a low performance of the solar cell,while conventional chemical doping always makes the films unstable and limits the scalability.In this work,for the first time,we simultaneously enhanced the hole transporting properties of P3HT film and the interface of perovskite by doping it with a judiciously designed oxidized small molecule organic semiconductor.The organic salt not only can promote the lamellar crystallinity of P3HT to obtain better charge transport properties,but also reduce the defects of perovskite.As a result,we achieved champion efficiencies of 23.0%for small-area solar cells and 18.8%for larger-area modules(48.0 cm^(2)).This efficiency is the highest value for P3HT-based perovskite modules.Moreover,the solar cells show excellent operational stability,retaining over 95%of their initial efficiencies after1200 h of continuous operation.展开更多
Developing efficient photocatalysts for CO_(2)conversion under full-spectrum irradiation remains a key challenge for solar-to-chemical energy conversion.In this study,a novel S-scheme heterojunction composed of reduct...Developing efficient photocatalysts for CO_(2)conversion under full-spectrum irradiation remains a key challenge for solar-to-chemical energy conversion.In this study,a novel S-scheme heterojunction composed of reduction Cs_(0.32)WO_(3)(CWO)nanosheets with hexagonal structure and oxidation WO_(3)·2H_(2)O(WO)nanorods with monoclinic structure photocatalyst was successfully constructed via an ultrasound strategy.Under full-spectrum irradiation for 4 h,the optimized 2D/1D of heterostructure CWO/WO-0.8 exhibited superior photocatalytic performance,achieving CO and CH_(3)OH yields of 29.74 and 63.71μmol·g^(-1),respectively.The enhanced activity is primarily ascribed to the formation of an S-scheme charge transfer pathway,which facilitates efficient separation and directional migration of photogenerated charge carriers through the internal electric field at the CWO/WO interface.This process facilitates the electron enrichment on the CWO surface and significantly enhances its CO_(2)reduction ability.Besides,the results of various characterizations show that CWO/WO-0.8 possesses enhanced optical response capability.The results of density functional theory calculations and CO_(2)-temperature programmed desorption analysis confirmed that the CWO/WO heterojunction exhibits stronger CO_(2)adsorption and activation abilities compared to the pristine CWO and WO.The reaction pathway for CH_(3)OH production was elucidated by in-situ diffused reflectance Fourier transformed infrared tests.This work provides new insights into the rational design of S-scheme photocatalysts for efficient and selective CO_(2)conversion.展开更多
The two-dimensional electron gas(2DEG)formed at the interface between two oxide insulators provides new opportunities for electronics and spintronics.The broken inversion symmetry at the heterointerface results in a R...The two-dimensional electron gas(2DEG)formed at the interface between two oxide insulators provides new opportunities for electronics and spintronics.The broken inversion symmetry at the heterointerface results in a Rashba spin-orbit coupling(RSOC)effect that enables the conversion between spin and charge currents.However,conducting oxide interfaces that simultaneously exhibit strong RSOC and high carrier mobility-a combination query for achieving high spin-to-charge inter-conversion efficiencies-remain scarce.Herein,we report a correlated 2DEG with giant Rashba splitting and high electron mobility in(111)-oriented EuTiO_(3)/KTaO_(3)(ETO/KTO)heterostructures under light illumination.Upon light modulation,a unique carrier-dependent giant anomalous Hall effect,the signature of spin-polarized 2DEG,emerges with a sign crossover at a carrier density of approximately 5.0×10^(13)cm^(-2),highlighting dramatic changes in the band topology of KTO(111)interface.Furthermore,at 2 K,the carrier mobility is enhanced from 103 cm^(2)·V^(-1)·s^(-1)to 1800 cm^(2)·V^(-1)·s^(-1),a remarkable enhancement of approximately 20 times.Accompanying with a giant Rashba coefficient αR up to 360meV·˚A,this high mobility ferromagnetic 5d oxide 2DEG is predicted to achieve a giant spin-to-charge conversion efficiency ofλ~10 nm,showing great potential for designing low-power spin-orbitronic devices.展开更多
Objective To develop a multimodal imaging atlas of a rat brain-computer interface(BCI)that incorporates brain,arterial,bone tissue and a BCI device using mixed reality(MR)for three-dimensional(3D)visualization.Methods...Objective To develop a multimodal imaging atlas of a rat brain-computer interface(BCI)that incorporates brain,arterial,bone tissue and a BCI device using mixed reality(MR)for three-dimensional(3D)visualization.Methods An invasive BCI was implanted in the left visual cortex of 4-week-old Sprague–Dawley rats.Multimodal imaging techniques,including micro-CT and 9.0 T MRI,were used to acquire images of the rat cranial bone structure,vascular distribution,brain tissue functional zones,and BCI device before and after implantation.Using 3D-slicer software,the images were fused through spatial transformations,followed by image segmentation and 3D model reconstruction.The HoloLens platform was employed for MR visualization.Results This study constructed a multimodal imaging atlas for rats that included the skull,brain tissue,arterial tissue,and BCI device coupled with MR technology to create an interactive 3D anatomical model.Conclusions This multimodal 3D atlas provides an objective and stable reference for exploring complex relationships between brain tissue structure and function,enhancing the understanding of the operational principles of BCIs.This is the first multimodal 3D imaging atlas related to a BCI created using Sprague–Dawley rats.展开更多
The current work addresses the challenge of elucidating the performance of fluoroelastomers within the HMX(octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine)based polymer-bonded explosives(PBXs).To simulate the confine...The current work addresses the challenge of elucidating the performance of fluoroelastomers within the HMX(octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine)based polymer-bonded explosives(PBXs).To simulate the confined interface in PBXs,bilayer films of F2314/HMX and F2311/HMX were designed.Neutron reflectivity(NR),nanoindentation,and X-ray reflectivity(XRR)were employed to examine the layer thickness,interface characteristics,diffusion behavior,and surface morphology of the bilayers.NR measurements revealed interface thicknesses of 45Å and 98Å for F2314/HMX and F2311/HMX,respectively,indicating deeper penetration of F2311 into the HMX matrix.NR also suggested a denser polymer network with a higher scattering length density(SLD)near the HMX interface for both fluoroelastomers,while the bound layer of F2311 was notably thicker.Nanoindentation cross-checks and confirms the presence of a bound layer,highlighting the differences in stiffness and diffusion ability between the two polymers.The consistency between the NR and nanoindentation results suggests that F2311 demonstrates better flexibility and elasticity,whereas F2314 is stiffer and more plastic.Accordingly,the structures and performances of different fluoroelastomers at the HMX interface are discussed,which can provide valuable insights into the selection of binders for PBX formulations tailored to specific applications.展开更多
All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices,while their application is still in the initial stage.Here,a metal halide doping strategy was implem...All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices,while their application is still in the initial stage.Here,a metal halide doping strategy was implemented to enhance device performance and stability for inverted CsPbI_(3)perovskite solar cells(PSCs),which are ideal for integration into perovskite/silicon tandem solar cells.The lanthanide compound terbium chloride(TbCl_(3))was employed to improve buried interface between[4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)and perovskite layer,thereby enhancing the crystallinity of CsPbI_(3)films and passivating non-radiative recombination defects.Thus,the inverted CsPbI_(3)PSCs achieved an efficiency of 18.68%and demonstrated excellent stability against water and oxygen.Meanwhile,remarkable efficiencies of 29.40%and 25.44%were,respectively,achieved in four-terminal(4T)and two-terminal(2T)perovskite/silicon mechanically tandem devices,which are higher efficiencies among reported all-inorganic perovskite-based tandem solar cells.This study presents a novel approach for fabricating highly efficient and stable inverted all-inorganic PSCs and perovskite/silicon tandem solar cells.展开更多
Bismuth oxyselenide(Bi_(2)O_(2)Se),a novel quasi-two-dimensional charge-carrying semiconductor,is recognized as one of the most promising emerging platforms for next-generation semiconductor devices.Recent advancement...Bismuth oxyselenide(Bi_(2)O_(2)Se),a novel quasi-two-dimensional charge-carrying semiconductor,is recognized as one of the most promising emerging platforms for next-generation semiconductor devices.Recent advancements in the development of diverse Bi_(2)O_(2)Se heterojunctions have unveiled extensive potential applications in both electronics and optoelectronics.However,achieving an in-depth understanding of band alignment and particularly interface dynamics remains a significant challenge.In this study,we conduct a comprehensive experimental investigation into band alignment utilizing high-resolution X-ray photoelectron spectroscopy(HRXPS),while also thoroughly discussing the properties of interface states.Our findings reveal that ultrathin films of Bi_(2)O_(2)Se grown on SrTiO_(3)(with TiO_(2)(001)termination)exhibit Type-I(straddling gap)band alignment characterized by a valence band offset(VBO)of approximately 1.77±0.04 eV and a conduction band offset(CBO)around 0.68±0.04 eV.Notably,when accounting for the influence of interface states,the bands at the interface display a herringbone configuration due to substantial built-in electric fields,which markedly deviate from conventional band alignments.Thus,our results provide valuable insights for advancing high-efficiency electronic and optoelectronic devices,particularly those where charge transfer is highly sensitive to interface states.展开更多
Electrochemical nitrate(NO_(3)^(-))reduction offers a promising route for ammonia(NH_(3))synthesis from industrial wastewater using renewable energy.However,achieving selective and active NO_(3)^(-)to NH_(3)conversion...Electrochemical nitrate(NO_(3)^(-))reduction offers a promising route for ammonia(NH_(3))synthesis from industrial wastewater using renewable energy.However,achieving selective and active NO_(3)^(-)to NH_(3)conversion at low potentials remains challenging due to complex multi-electron transfer processes and competing reactions.Herein,we tackle this challenge by developing a cascade catalysis approach using synergistic active sites at Cu-Fe_(2)O_(3)interfaces,significantly reducing the NO_(3)^(-)to NH_(3)at a low onset potential to about+0.4 V_(RHE).Specifically,Cu optimizes^(*)NO_(3)adsorption,facilitating NO_(3)^(-)to nitrite(NO_(2)-)conversion,while adjacent Fe species in Fe_(2)O_(3)promote the subsequent NO_(2)-reduction to NH_(3)with favorable^(*)NO_(2)adsorption.Electrochemical operating experiments,in situ Raman spectroscopy,and in situ infrared spectroscopy consolidate this improved onset potential and reduction kinetics via cascade catalysis.An NH_(3)partial current density of~423 mA cm^(-2)and an NH_(3)Faradaic efficiency(FENH_(3))of 99.4%were achieved at-0.6 V_(RHE),with a maximum NH_(3)production rate of 2.71 mmol h^(-1)cm^(-2)at-0.8 V_(RHE).Remarkably,the half-cell energy efficiency exceeded 35%at-0.27 V_(RHE)(80%iR corrected),maintaining an FENH_(3)above 90%across a wide range of NO_(3)^(-)concentrations(0.05^(-1)mol L^(-1)).Using 15N isotopic tracing,we confirmed NO_(3)^(-)as the sole nitrogen source and attained a 98%NO_(3)^(-)removal efficiency.The catalyst exhibit stability over 106-h of continuous operation without noticeable degradation.This work highlights distinctive active sites in Cu-Fe_(2)O_(3)for promoting the cascade NO_(3)^(-)to NO_(2)^(-)and NO_(2)^(-)to NH_(3)electrolysis at industrial relevant current densities.展开更多
Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.L...Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.Li^(+)/Li)constrains their use in ultrahighvoltage systems(e.g.,4.8 V).In this work,ferroelectric Ba TiO_(3)(BTO)nanoparticles with optimized thickness of~50-100 nm were successfully coated onto Li_(2.5)Y_(0.5)Zr_(0.5)Cl_(6)(LYZC@5BTO)electrolytes using a time-efficient ball-milling process.The nanoparticle-induced interfacial ionic conduction enhancement mechanism contributed to the preservation of LYZC’s high ionic conductivity,which remained at 1.06 m S cm^(-1)for LYZC@5BTO.Furthermore,this surface electric field engineering strategy effectively mitigates the voltage-induced self-decomposition of chloride-based solid electrolytes,suppresses parasitic interfacial reactions with single-crystal NCM811(SCNCM811),and inhibits the irreversible phase transition of SCNCM811.Consequently,the cycling stability of LYZC under high-voltage conditions(4.8 V vs.Li+/Li)is significantly improved.Specifically,ASSB cells employing LYZC@5BTO exhibited a superior discharge capacity of 95.4 m Ah g^(-1)over 200 cycles at 1 C,way outperforming cell using pristine LYZC that only shows a capacity of 55.4 m Ah g^(-1).Furthermore,time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy analysis revealed that Metal-O-Cl by-products from cumulative interfacial side reactions accounted for 6% of the surface species initially,rising to 26% after 200 cycles in pristine LYZC.In contrast,LYZC@5BTO limited this increase to only 14%,confirming the effectiveness of BTO in stabilizing the interfacial chemistry.This electric field modulation strategy offers a promising route toward the commercialization of high-voltage solid-state electrolytes and energy-dense ASSBs.展开更多
文摘Invasive as well as non-invasive neurotechnologies conceptualized to interface the central and peripheral nervous system have been probed for the past decades,which refer to electroencephalography,electrocorticography and microelectrode arrays.The challenges of these mentioned approaches are characterized by the bandwidth of the spatiotemporal resolution,which in turn is essential for large-area neuron recordings(Abiri et al.,2019).
基金supported by the National Natural Science Foundation of China(Nos.52122408 and 52474397)the High-level Talent Research Start-up Project Funding of Henan Academy of Sciences(No.242017127)+1 种基金the financial support from the Fundamental Research Funds for the Central Universities(University of Science and Technology Beijing(USTB),Nos.FRF-TP-2021-04C1 and 06500135)supported by USTB MatCom of Beijing Advanced Innovation Center for Materials Genome Engineering。
文摘High-performance alloys are indispensable in modern engineering because of their exceptional strength,ductility,corrosion resistance,fatigue resistance,and thermal stability,which are all significantly influenced by the alloy interface structures.Despite substantial efforts,a comprehensive overview of interface engineering of high-performance alloys has not been presented so far.In this study,the interfaces in high-performance alloys,particularly grain and phase boundaries,were systematically examined,with emphasis on their crystallographic characteristics and chemical element segregations.The effects of the interfaces on the electrical conductivity,mechanical strength,toughness,hydrogen embrittlement resistance,and thermal stability of the alloys were elucidated.Moreover,correlations among various types of interfaces and advanced experimental and computational techniques were examined using big data analytics,enabling robust design strategies.Challenges currently faced in the field of interface engineering and emerging opportunities in the field are also discussed.The study results would guide the development of next-generation high-performance alloys.
基金supported by Guangdong Major Project of Basic and Applied Basic Research, China (No. 2020B0301030006)Fundamental Research Funds for the Central Universities, China (No. SWU-XDJH202313)+1 种基金Chongqing Postdoctoral Science Foundation Funded Project, China (No. 2112012728014435)the Chongqing Postgraduate Research and Innovation Project, China (No. CYS23197)。
文摘A new method was proposed for preparing AZ31/1060 composite plates with a corrugated interface,which involved cold-pressing a corrugated surface on the Al plate and then hot-pressing the assembled Mg/Al plate.The results show that cold-pressing produces intense plastic deformation near the corrugated surface of the Al plate,which promotes dynamic recrystallization of the Al substrate near the interface during the subsequent hot-pressing.In addition,the initial corrugation on the surface of the Al plate also changes the local stress state near the interface during hot pressing,which has a large effect on the texture components of the substrates near the corrugated interface.The construction of the corrugated interface can greatly enhance the shear strength by 2−4 times due to the increased contact area and the strong“mechanical gearing”effect.Moreover,the mechanical properties are largely depended on the orientation relationship between corrugated direction and loading direction.
基金the financial support from the National Natural Science Foundation of China(52203123 and 52473248)State Key Laboratory of Polymer Materials Engineering(sklpme2024-2-04)+1 种基金the Fundamental Research Funds for the Central Universitiessponsored by the Double First-Class Construction Funds of Sichuan University。
文摘Composite polymer electrolytes(CPEs)offer a promising solution for all-solid-state lithium-metal batteries(ASSLMBs).However,conventional nanofillers with Lewis-acid-base surfaces make limited contribution to improving the overall performance of CPEs due to their difficulty in achieving robust electrochemical and mechanical interfaces simultaneously.Here,by regulating the surface charge characteristics of halloysite nanotube(HNT),we propose a concept of lithium-ion dynamic interface(Li^(+)-DI)engineering in nano-charged CPE(NCCPE).Results show that the surface charge characteristics of HNTs fundamentally change the Li^(+)-DI,and thereof the mechanical and ion-conduction behaviors of the NCCPEs.Particularly,the HNTs with positively charged surface(HNTs+)lead to a higher Li^(+)transference number(0.86)than that of HNTs-(0.73),but a lower toughness(102.13 MJ m^(-3)for HNTs+and 159.69 MJ m^(-3)for HNTs-).Meanwhile,a strong interface compatibilization effect by Li^(+)is observed for especially the HNTs+-involved Li^(+)-DI,which improves the toughness by 2000%compared with the control.Moreover,HNTs+are more effective to weaken the Li^(+)-solvation strength and facilitate the formation of Li F-rich solid-electrolyte interphase of Li metal compared to HNTs-.The resultant Li|NCCPE|LiFePO4cell delivers a capacity of 144.9 m Ah g^(-1)after 400 cycles at 0.5 C and a capacity retention of 78.6%.This study provides deep insights into understanding the roles of surface charges of nanofillers in regulating the mechanical and electrochemical interfaces in ASSLMBs.
基金supported by the National Natural Science Foundation of China (No. 52374292)China Baowu Low Carbon Metallurgy Innovation Foundation, China (No. BWLCF202309)the Natural Science Foundation of Changsha City, China (No. KQ2208271)。
文摘Some active metal oxides(Al_(2)O_(3),TiO_(2),and Cr_(2)O_(3))were selected as dopants to the Al_(2)O_(3)-based ceramic shells for investment casting of K417G superalloy.The effects of dopant types and contents(0,2,5,and 8 wt.%)on the wettability and interfacial reaction between the alloy and shell were investigated by a sessile-drop experiment.The results show that increasing the Al_(2)O_(3) doping contents(0−8 wt.%)reduces the porosity(21.74%−10.08%)and roughness(3.22−1.34μm)of the shell surface.The increase in Cr_(2)O_(3) dopant content(2−8 wt.%)further exacerbates the interfacial reaction,leading to an increase in the thickness of the reaction layer(2.6−3.1μm)and a decrease in the wetting angle(93.9°−91.0°).The addition of Al_(2)O_(3) and TiO_(2) dopants leads to the formation of Al_(2)TiO_(5) composite oxides in the reaction products,which effectively inhibits the interfacial reaction.The increase in TiO_(2) dopant contents(0−8 wt.%)further promotes the formation of Al_(2)TiO_(5),which decreases the thickness of the interfacial reaction layer(3.9−1.2μm)and increases the wetting angle(95.0°−103.8°).The introduced dopants enhance the packing density of the shell surface,while simultaneously suppress the diffusion of active metal elements from the alloy matrix to the interface.
基金supported by the National Natural Science Foundation of China(No.22209073 to Z.H.L.)the Natural Science Foundation of Jiangsu Province(No.BK20220912 to Z.H.L.)+3 种基金the Science the Technology Innovation Fund for Emission Peak and Carbon Neutrality of Jiangsu province(No.BK20231512 to M.B.Z.)the National Natural Science Foundation of China(No.52072173 to L.F.S.)International Science and Technology Cooperation Program of Jiangsu Province(No.SBZ2022000084 to L.F.S.)the Fundamental Research Funds for the Central Universities(Nos.ILA22061 and ILA22075 to L.F.S.).
文摘The O3-type NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(NFM)has emerged as a highly promising cathode material for sodiumion batteries due to its facile synthesis and high theoretical capacity.However,it suffers from severe capacity and rate capability degradation caused by multiple coupled failure mechanisms,including irreversible phase transitions,structural deterioration at high voltages,and electrolyte-induced surface corrosion.This work addresses the challenge of high-voltage stability in NFM cathodes via a synergistic bulk-phase and interface engineering strategy.Firstly,Li,Ti,and Co are codoped into the bulk lattice structure to suppress the Mn^(3+)-induced Jahn-Teller distortion and improve Na^(+)diffusion kinetics.And then,an AlPO_(4) protective coating layer is fabricated to mitigate electrolyte corrosion and interfacial side reactions.Consequently,the as-designed composite cathode(AP@NFMLTC)can effectively suppress the P3 to O3’phase transition within the voltage range of 2.0 to 4.2 V,resulting in a highly reversible sodium storage mechanism.After 100 cycles at a rate of 1 C,the capacity retention rate significantly improves from 45.6%to 83.6%,with a minimal voltage decay of just 0.08 V.The dual bulk-interface synergistic strategy in this work provides valuable insights into achieving high stable operation for sodium-ion batteries(SIBs)cathodes under enhanced voltage.
文摘Practical application of Na_(3)SbS_(4)(NSS)solid-state electrolyte in sodium metal batteries has been significantly hindered by poor interfacial stability and insufficient ionic conductivity.In this study,a series of dual-site doped Na_(3-2x)Sb_(1-x)W_(x)S_(4-x)F_(x)(x=0,0.12,0.24,0.36)electrolytes through high-energy ball milling followed by high-temperature sintering is prepared,where tungsten(W)substitutes for antimony(Sb)and fluorine(F)replaces sulfur(S)in the NSS lattice.The co-doping of W and F not only broadens the interplanar spacing of NSS but also promotes the stable formation of the cubic phase of NSS,thereby effectively enhancing the transport ability of sodium ions within NSS.Among them,Na_(2.52)Sb_(0.76)W_(0.24)S_(3.76)F_(0.24) exhibits the highest ionic conductivity of 4.45 mS·cm^(-1).Furthermore,F doping facilitates the in-situ formation of NaF between the electrolyte and metallic sodium,significantly improving interfacial stability.Electrochemical evaluation shows that the Na/Na_(2.52)Sb_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na symmetric cell achieves a high critical current density of 1.65 mA·cm^(-2) and maintains stable sodium plating/stripping cycling for 500 h at 0.1 mA·cm^(-2).Additionally,the TiS2/Na_(2.52)Sb_(0.76)W_(0.24)S_(3.76)F_(0.24)/Na full cell exhibits outstanding cycling stability and rate capability.
基金supported by the National Natural Science Foundation of China(Nos.22173057,52130204,12074241,11929401,12311530675)Science and Technology Commission of Shanghai Municipality(Nos.21JC1402700,22XD1400900,20501130600,21JC1402600)High-Performance Computing Center,Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University。
文摘Metal-ceramic composites combine the excellent properties of metals and ceramics,which have high strength,stability,and corrosion re-sistance.Al_(2)O_(3)/FeCo composites have been proven to be useful in ap-plications such as catalysts,mi-crowave absorption materials,and enhanced permeability dielectric.The understanding of the mechani-cal properties and dynamics at the atomic scale of the Al_(2)O_(3)/FeCo in-terface can promote the design and exploitment of metal-ceramic composites.In this work,we have obtained Young’s modulus and diffusion coefficient of the Al_(2)O_(3)/FeCo interface using molecular dynamics simulation,elucidated the structural characteristics of the Al_(2)O_(3)/FeCo interface at the atomic scale,and investigated the impact of atomic magnetism and the exter-nal magnetic field on the interface.Simulated results show that Young’s modulus of the Al_(2)O_(3)/FeCo interface is significantly improved compared with pure Al_(2)O_(3)and FeCo alloy at room and high temperatures.When the atomic magnetism and the external magnetic field are applied,Young’s modulus of the Al_(2)O_(3)/FeCo interface further increases to 612 GPa at 300 K and 602 GPa at 500 K.Moreover,the average density,diffusion coefficient,and radial distri-bution function are found to be modified substantially.This study will shed light on the atom-istic investigations of the metal-ceramic composites.
基金supported by the National Natural Science Foundation of China(Nos.62304171 and 62374128)the China Postdoctoral Science Foundation(No.2022M722500)+2 种基金the Key Research and Development Program of Shaanxi Province(No.2024GX-YBXM-512)Xidian University Specially Funded Project for Interdisciplinary Exploration(Nos.TZJH2024052 and TZJH2024050)the Fundamental Research Funds for the Central Universities,the open fund of State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology(No.2024-KF-12).
文摘CsPbBr_(3)perovskite solar cells(PSCs)have attracted significant interest for their remarkable stability under high temperatures and humidity.However,challenges such as energy loss at the CsPbBr_(3)/oxide buried interface and imperfect band alignment have impeded further efficiency enhancements.In this study,TiO_(2),SnO_(2),or ZnO was employed as electron transport layer(ETL)materials,respectively,in CsPbBr_(3)-based PSCs to optimize the band alignment at the ETL/CsPbBr_(3)interface and enhance the film quality of CsPbBr_(3)materials.The research findings indicate that the power conversion efficiency(PCE)of PSCs is influenced by the choice of ETL material.Specifically,TiO_(2)-based PSCs achieved a PCE of 10.37%efficiency,higher than SnO_(2)-or ZnO-based PSCs.This disparity in PCE can be attributed to variations in open-circuit voltage,which stem from different band alignments at the ETL/CsPbBr_(3)interface.Notably,superior photovoltaic performance was consistently observed in TiO_(2)-based PSCs due to the substantial conduction band offset(∆Ec)at the TiO_(2)/CsPbBr_(3)interface and the high quality of the CsPbBr_(3)film.This not only enhances electron extraction at the TiO_(2)/CsPbBr_(3)interface but also diminishes non-radiative recombination at the interface,as confirmed by density functional theory(DFT)calculations and experiments.Furthermore,photodetectors(PDs)based on TiO_(2)/CsPbBr_(3)heterojunction exhibit high photoresponse and photodetectivity.In conclusion,this study underscores the critical importance of the buried interface contact in CsPbBr_(3)and offers a direct approach for fabricating efficient and stable inorganic PSCs and PDs.
基金financial support provided by the Sichuan Science and Technology Program(No.2022NSFSC0226)Sichuan Science and Technology Program(No.2023ZYD0163)+6 种基金the Production-Education Integration Demonstration Project of Sichuan Provincethe Photovoltaic Industry Production-Education Integration Comprehensive Demonstration Base of Sichuan Province(Sichuan Financial Education[2022]No.106)China Tianfu Yongxing Laboratory Science and Technology Key Project(2023KJGG15)National Key Research and Development Program of China(2022YFB3803300)Beijing Natural Science Foundation(IS23037)the Department for Energy Security and Net Zero(project ID:NEXTCCUS)the ACT program(Accelerating CCS Technologies,Horizon2020 project NO.691712)。
文摘The 2D/3D heterojunction perovskites have garnered increasing attention due to their exceptional moisture and thermal stability.However,few works have paid attention to the influence of the subsequent change process of 2D/3D heterojunction PSC on the stability of PSCs.Moreover,the evolution of the interface and carrier dynamic behavior of the 2D/3D perovskite films with long-term operation has not been systematically developed befo re.In this work,the effects of 2D/3 D heterojunction evolution on the interface of perovskite films and different carrier dynamics during 2D/3D evolution are systematically analyzed for the first time.The decomposition of 2D/3D heterojunction in the perovskite film will have a certain impact on the surface and carrier dynamics behavior of perovskite.During the evolution of 2D/3D heterojunction,PbI_(2)crystals will appear,which will improve the interfacial energy level matching between the electron transport layer and perovskite film.With a long evolution time,some holes will appear on the surface of perovskite film.The open circuit voltage(V_(OC))of PSCs increased from 1.14 to1.18 V and the PCE increased to 23.21%after 300 h storage in the nitrogen atmosphere,and maintained 89%initial performance for with 3000 h stability test in N_(2)box.This discovery has a significant role in promoting the development of inverted heterojunction PSCs and constructing the revolution mechanism of charge carrier dynamic.
基金financially supported by the National Natural Science Foundation of China(52472248 and 22075221)the Key Research and Development Project of Shanxi Province(202202060301003 and 202202060301015)the Innovation Program of Wuhan-Shuguang Project(2023010201020367)。
文摘Poly(3-hexylthiophene)(P3HT)is one of the most promising hole-transporting materials in the pursuit of efficient and stable perovskite solar cells due to its outstanding stability and low cost.However,the intrinsic low carrier density of P3 HT and poor contact between the P3HT/perovskite interface always lead to a low performance of the solar cell,while conventional chemical doping always makes the films unstable and limits the scalability.In this work,for the first time,we simultaneously enhanced the hole transporting properties of P3HT film and the interface of perovskite by doping it with a judiciously designed oxidized small molecule organic semiconductor.The organic salt not only can promote the lamellar crystallinity of P3HT to obtain better charge transport properties,but also reduce the defects of perovskite.As a result,we achieved champion efficiencies of 23.0%for small-area solar cells and 18.8%for larger-area modules(48.0 cm^(2)).This efficiency is the highest value for P3HT-based perovskite modules.Moreover,the solar cells show excellent operational stability,retaining over 95%of their initial efficiencies after1200 h of continuous operation.
文摘Developing efficient photocatalysts for CO_(2)conversion under full-spectrum irradiation remains a key challenge for solar-to-chemical energy conversion.In this study,a novel S-scheme heterojunction composed of reduction Cs_(0.32)WO_(3)(CWO)nanosheets with hexagonal structure and oxidation WO_(3)·2H_(2)O(WO)nanorods with monoclinic structure photocatalyst was successfully constructed via an ultrasound strategy.Under full-spectrum irradiation for 4 h,the optimized 2D/1D of heterostructure CWO/WO-0.8 exhibited superior photocatalytic performance,achieving CO and CH_(3)OH yields of 29.74 and 63.71μmol·g^(-1),respectively.The enhanced activity is primarily ascribed to the formation of an S-scheme charge transfer pathway,which facilitates efficient separation and directional migration of photogenerated charge carriers through the internal electric field at the CWO/WO interface.This process facilitates the electron enrichment on the CWO surface and significantly enhances its CO_(2)reduction ability.Besides,the results of various characterizations show that CWO/WO-0.8 possesses enhanced optical response capability.The results of density functional theory calculations and CO_(2)-temperature programmed desorption analysis confirmed that the CWO/WO heterojunction exhibits stronger CO_(2)adsorption and activation abilities compared to the pristine CWO and WO.The reaction pathway for CH_(3)OH production was elucidated by in-situ diffused reflectance Fourier transformed infrared tests.This work provides new insights into the rational design of S-scheme photocatalysts for efficient and selective CO_(2)conversion.
基金supported by the Science Center of the National Science Foundation of China(Grant No.52088101)the National Key Research and Development Program of China(Grant Nos.2023YFA1406400,2021YFA1400300,and 2023YFA1607403)the National Natural Science Foundation of China(Grant Nos.T2394472 and T2394470).
文摘The two-dimensional electron gas(2DEG)formed at the interface between two oxide insulators provides new opportunities for electronics and spintronics.The broken inversion symmetry at the heterointerface results in a Rashba spin-orbit coupling(RSOC)effect that enables the conversion between spin and charge currents.However,conducting oxide interfaces that simultaneously exhibit strong RSOC and high carrier mobility-a combination query for achieving high spin-to-charge inter-conversion efficiencies-remain scarce.Herein,we report a correlated 2DEG with giant Rashba splitting and high electron mobility in(111)-oriented EuTiO_(3)/KTaO_(3)(ETO/KTO)heterostructures under light illumination.Upon light modulation,a unique carrier-dependent giant anomalous Hall effect,the signature of spin-polarized 2DEG,emerges with a sign crossover at a carrier density of approximately 5.0×10^(13)cm^(-2),highlighting dramatic changes in the band topology of KTO(111)interface.Furthermore,at 2 K,the carrier mobility is enhanced from 103 cm^(2)·V^(-1)·s^(-1)to 1800 cm^(2)·V^(-1)·s^(-1),a remarkable enhancement of approximately 20 times.Accompanying with a giant Rashba coefficient αR up to 360meV·˚A,this high mobility ferromagnetic 5d oxide 2DEG is predicted to achieve a giant spin-to-charge conversion efficiency ofλ~10 nm,showing great potential for designing low-power spin-orbitronic devices.
基金supported by the National Natural Science Foundation of China(No.82172524 and No.81974355)National Innovation Platform Development Program(No.2020021105012440),China+3 种基金Major Program of Hubei Province(No.2021BEA161),ChinaMajor Key Project of Hubei Province(No.JD2023BAA005),ChinaWuhan Union Hospital Free Innovation Preliminary Research Fund(No.2024XHYN047),ChinaJoint Funds for the Innovation of Science and Technology(No.2024Y9062),Fujian Province,China.
文摘Objective To develop a multimodal imaging atlas of a rat brain-computer interface(BCI)that incorporates brain,arterial,bone tissue and a BCI device using mixed reality(MR)for three-dimensional(3D)visualization.Methods An invasive BCI was implanted in the left visual cortex of 4-week-old Sprague–Dawley rats.Multimodal imaging techniques,including micro-CT and 9.0 T MRI,were used to acquire images of the rat cranial bone structure,vascular distribution,brain tissue functional zones,and BCI device before and after implantation.Using 3D-slicer software,the images were fused through spatial transformations,followed by image segmentation and 3D model reconstruction.The HoloLens platform was employed for MR visualization.Results This study constructed a multimodal imaging atlas for rats that included the skull,brain tissue,arterial tissue,and BCI device coupled with MR technology to create an interactive 3D anatomical model.Conclusions This multimodal 3D atlas provides an objective and stable reference for exploring complex relationships between brain tissue structure and function,enhancing the understanding of the operational principles of BCIs.This is the first multimodal 3D imaging atlas related to a BCI created using Sprague–Dawley rats.
基金supported in part by the National Natural Science Foundation of China(Nos.12335018,12105264,and 12275248)NSAF Joint Fund Project(Nos.U2230107,U1730244,U2130207)+1 种基金Innovation and Development Fund of China Academy of Engineering Physics(No.CXKS20240052)Central Guidance for Local Science and Technology Development Fund Project(No.2023ZYDF075).
文摘The current work addresses the challenge of elucidating the performance of fluoroelastomers within the HMX(octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine)based polymer-bonded explosives(PBXs).To simulate the confined interface in PBXs,bilayer films of F2314/HMX and F2311/HMX were designed.Neutron reflectivity(NR),nanoindentation,and X-ray reflectivity(XRR)were employed to examine the layer thickness,interface characteristics,diffusion behavior,and surface morphology of the bilayers.NR measurements revealed interface thicknesses of 45Å and 98Å for F2314/HMX and F2311/HMX,respectively,indicating deeper penetration of F2311 into the HMX matrix.NR also suggested a denser polymer network with a higher scattering length density(SLD)near the HMX interface for both fluoroelastomers,while the bound layer of F2311 was notably thicker.Nanoindentation cross-checks and confirms the presence of a bound layer,highlighting the differences in stiffness and diffusion ability between the two polymers.The consistency between the NR and nanoindentation results suggests that F2311 demonstrates better flexibility and elasticity,whereas F2314 is stiffer and more plastic.Accordingly,the structures and performances of different fluoroelastomers at the HMX interface are discussed,which can provide valuable insights into the selection of binders for PBX formulations tailored to specific applications.
基金the financial support from the National Natural Science Foundation of China(62274132,62204189,62274126)the Postdoctoral Fellowship Program of CPSF(GZC20241301)+1 种基金Fundamental Research Funds for the Central Universities(ZYTS25221)the National Key R&D Program of China(2022YFB3605402,2021YFF0500501)。
文摘All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices,while their application is still in the initial stage.Here,a metal halide doping strategy was implemented to enhance device performance and stability for inverted CsPbI_(3)perovskite solar cells(PSCs),which are ideal for integration into perovskite/silicon tandem solar cells.The lanthanide compound terbium chloride(TbCl_(3))was employed to improve buried interface between[4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)and perovskite layer,thereby enhancing the crystallinity of CsPbI_(3)films and passivating non-radiative recombination defects.Thus,the inverted CsPbI_(3)PSCs achieved an efficiency of 18.68%and demonstrated excellent stability against water and oxygen.Meanwhile,remarkable efficiencies of 29.40%and 25.44%were,respectively,achieved in four-terminal(4T)and two-terminal(2T)perovskite/silicon mechanically tandem devices,which are higher efficiencies among reported all-inorganic perovskite-based tandem solar cells.This study presents a novel approach for fabricating highly efficient and stable inverted all-inorganic PSCs and perovskite/silicon tandem solar cells.
基金supported by the National Natural Science Foundation of China(Nos.52072059,12304078,12274061 and 11774044)the Natural Science Foundation of Sichuan Province(No.2024NSFSC1384).
文摘Bismuth oxyselenide(Bi_(2)O_(2)Se),a novel quasi-two-dimensional charge-carrying semiconductor,is recognized as one of the most promising emerging platforms for next-generation semiconductor devices.Recent advancements in the development of diverse Bi_(2)O_(2)Se heterojunctions have unveiled extensive potential applications in both electronics and optoelectronics.However,achieving an in-depth understanding of band alignment and particularly interface dynamics remains a significant challenge.In this study,we conduct a comprehensive experimental investigation into band alignment utilizing high-resolution X-ray photoelectron spectroscopy(HRXPS),while also thoroughly discussing the properties of interface states.Our findings reveal that ultrathin films of Bi_(2)O_(2)Se grown on SrTiO_(3)(with TiO_(2)(001)termination)exhibit Type-I(straddling gap)band alignment characterized by a valence band offset(VBO)of approximately 1.77±0.04 eV and a conduction band offset(CBO)around 0.68±0.04 eV.Notably,when accounting for the influence of interface states,the bands at the interface display a herringbone configuration due to substantial built-in electric fields,which markedly deviate from conventional band alignments.Thus,our results provide valuable insights for advancing high-efficiency electronic and optoelectronic devices,particularly those where charge transfer is highly sensitive to interface states.
文摘Electrochemical nitrate(NO_(3)^(-))reduction offers a promising route for ammonia(NH_(3))synthesis from industrial wastewater using renewable energy.However,achieving selective and active NO_(3)^(-)to NH_(3)conversion at low potentials remains challenging due to complex multi-electron transfer processes and competing reactions.Herein,we tackle this challenge by developing a cascade catalysis approach using synergistic active sites at Cu-Fe_(2)O_(3)interfaces,significantly reducing the NO_(3)^(-)to NH_(3)at a low onset potential to about+0.4 V_(RHE).Specifically,Cu optimizes^(*)NO_(3)adsorption,facilitating NO_(3)^(-)to nitrite(NO_(2)-)conversion,while adjacent Fe species in Fe_(2)O_(3)promote the subsequent NO_(2)-reduction to NH_(3)with favorable^(*)NO_(2)adsorption.Electrochemical operating experiments,in situ Raman spectroscopy,and in situ infrared spectroscopy consolidate this improved onset potential and reduction kinetics via cascade catalysis.An NH_(3)partial current density of~423 mA cm^(-2)and an NH_(3)Faradaic efficiency(FENH_(3))of 99.4%were achieved at-0.6 V_(RHE),with a maximum NH_(3)production rate of 2.71 mmol h^(-1)cm^(-2)at-0.8 V_(RHE).Remarkably,the half-cell energy efficiency exceeded 35%at-0.27 V_(RHE)(80%iR corrected),maintaining an FENH_(3)above 90%across a wide range of NO_(3)^(-)concentrations(0.05^(-1)mol L^(-1)).Using 15N isotopic tracing,we confirmed NO_(3)^(-)as the sole nitrogen source and attained a 98%NO_(3)^(-)removal efficiency.The catalyst exhibit stability over 106-h of continuous operation without noticeable degradation.This work highlights distinctive active sites in Cu-Fe_(2)O_(3)for promoting the cascade NO_(3)^(-)to NO_(2)^(-)and NO_(2)^(-)to NH_(3)electrolysis at industrial relevant current densities.
基金financially supported by Shenzhen Science and Technology Program(JCYJ20240813142900001)Guangdong Provincial Key Laboratory of New Energy Materials Service Safety。
文摘Chloride-based solid electrolytes are considered promising candidates for next-generation high-energy-density all-solid-state batteries(ASSBs).However,their relatively low oxidative decomposition threshold(~4.2 V vs.Li^(+)/Li)constrains their use in ultrahighvoltage systems(e.g.,4.8 V).In this work,ferroelectric Ba TiO_(3)(BTO)nanoparticles with optimized thickness of~50-100 nm were successfully coated onto Li_(2.5)Y_(0.5)Zr_(0.5)Cl_(6)(LYZC@5BTO)electrolytes using a time-efficient ball-milling process.The nanoparticle-induced interfacial ionic conduction enhancement mechanism contributed to the preservation of LYZC’s high ionic conductivity,which remained at 1.06 m S cm^(-1)for LYZC@5BTO.Furthermore,this surface electric field engineering strategy effectively mitigates the voltage-induced self-decomposition of chloride-based solid electrolytes,suppresses parasitic interfacial reactions with single-crystal NCM811(SCNCM811),and inhibits the irreversible phase transition of SCNCM811.Consequently,the cycling stability of LYZC under high-voltage conditions(4.8 V vs.Li+/Li)is significantly improved.Specifically,ASSB cells employing LYZC@5BTO exhibited a superior discharge capacity of 95.4 m Ah g^(-1)over 200 cycles at 1 C,way outperforming cell using pristine LYZC that only shows a capacity of 55.4 m Ah g^(-1).Furthermore,time-of-flight secondary ion mass spectrometry and X-ray photoelectron spectroscopy analysis revealed that Metal-O-Cl by-products from cumulative interfacial side reactions accounted for 6% of the surface species initially,rising to 26% after 200 cycles in pristine LYZC.In contrast,LYZC@5BTO limited this increase to only 14%,confirming the effectiveness of BTO in stabilizing the interfacial chemistry.This electric field modulation strategy offers a promising route toward the commercialization of high-voltage solid-state electrolytes and energy-dense ASSBs.
