Heterointerfaces have been pivotal in unveiling extraordinary interfacial properties and enabling multifunctional material platforms.Despite extensive research on all-oxide interfaces,heterointerfaces between differen...Heterointerfaces have been pivotal in unveiling extraordinary interfacial properties and enabling multifunctional material platforms.Despite extensive research on all-oxide interfaces,heterointerfaces between different material classes,such as oxides and nitrides,remain underexplored.Here we present the fabrication of atomically sharp heterointerfaces between antiperovskite Ni_(3)InN and perovskite SrVO_(3).Leveraging layer-resolved scanning transmission electron microscopy and electron energy loss spectroscopy,we identified pronounced charge transfer across the well-ordered interface.First-principles calculations confirmed our experimental observations and further predicted an emergent magnetic moment within the Ni_(3)InN layer due to the charge transfer.These findings pave the way for novel electronic and spintronic applications by enabling tunable interfacial properties in nitride/oxide systems.展开更多
Gradient magnetic heterointerfaces have injected infinite vitality in optimizing impedance matching,adjusting dielectric/magnetic resonance and promoting electromagnetic(EM)wave absorption,but still exist a significan...Gradient magnetic heterointerfaces have injected infinite vitality in optimizing impedance matching,adjusting dielectric/magnetic resonance and promoting electromagnetic(EM)wave absorption,but still exist a significant challenging in regulating local phase evolution.Herein,accordion-shaped Co/Co_(3)O_(4)@N-doped carbon nanosheets(Co/Co_(3)O_(4)@NC)with gradient magnetic heterointerfaces have been fabricated via the cooperative high-temperature carbonization and lowtemperature oxidation process.The results indicate that the surface epitaxial growth of crystal Co_(3)O_(4) domains on local Co nanoparticles realizes the adjustment of magnetic-heteroatomic components,which are beneficial for optimizing impedance matching and interfacial polarization.Moreover,gradient magnetic heterointerfaces simultaneously realize magnetic coupling,and long-range magnetic diffraction.Specifically,the synthesized Co/Co_(3)O_(4)@NC absorbents display the strong electromagnetic wave attenuation capability of−53.5 dB at a thickness of 3.0 mm with an effective absorption bandwidth of 5.36 GHz,both are superior to those of single magnetic domains embedded in carbon matrix.This design concept provides us an inspiration in optimizing interfacial polarization,regulating magnetic coupling and promoting electromagnetic wave absorption.展开更多
The existence of multiple vacancies leads to significant changes in the local atomic structure,which can regulate the electronic structure of the surface and form unsaturated coordination geometries.However,the curren...The existence of multiple vacancies leads to significant changes in the local atomic structure,which can regulate the electronic structure of the surface and form unsaturated coordination geometries.However,the current methods employed to generate multiple vacancies in two-dimensional(2D)layered double hydroxide(LDH)materials are still difficult to achieve to some extent and are primarily limited to monolayer LDH structures.Here,we present an improved method to synthesize NiMoP/Ni_(2)P catalysts with a sponge-like porous structure.Firstly,NiO with dual defects was constructed by subjecting NiMo-LDH/Ni to air calcination.Subsequently,we performed phosphorization treatment and introduced multiple Ni vacancies and O vacancies as defect sites to tune the edge and substrate surfaces of LDH.At the same time,the electronic structure was tuned by adding P heteroatoms.The synergistic effect of porous structure,heterogeneous interfaces,vacancies,doping defects,and amorphous states can greatly enhance the electron transfer effect inside the catalysts,which significantly improves the catalytic ability of the oxygen evolution reaction(OER).Therefore,the overpotential for the oxygen evolution reaction of NiMoP/Ni_(2)P heterointerfaces reaches 270 mV at a current density of 10 mA·cm^(-2)under alkaline conditions,with the catalysts capable of sustaining high current densities even after the durability testing for 35 h.展开更多
Solvated zinc ions are prone to undergo desolvation at the electrode/electrolyte interfaces,and unstable H_(2)O molecules within the solvated sheaths tend to trigger hydrogen evolution reaction(HER),further accelerati...Solvated zinc ions are prone to undergo desolvation at the electrode/electrolyte interfaces,and unstable H_(2)O molecules within the solvated sheaths tend to trigger hydrogen evolution reaction(HER),further accelerating interfaces decay.Herein,we propose for the first time a novel strategy to enhance the interfacial stabilities by insitu dynamic reconstruction of weakly solvated Zn2þduring the desolvation processes at heterointerfaces.Theoretical calculations indicate that,due to built-in electric field effects(BEFs),the plating/stripping mechanism shifts from[Zn(H_(2)O)_(6)]_(2)þto[Zn(H_(2)O)_(5)(SO_(4))^(2-)]_(2)þwithout additional electrolyte additives,reducing the solvation ability of H_(2)O,enhancing the competitive coordination of SO_(4)^(2-),essentially eliminating the undesirable side effects of anodes.Hence,symmetric cells can operate stably for 3000 h(51.7-times increase in cycle life),and the full cells can operate stably for 5000 cycles(51.5-times increase in cycle life).This study provides valuable insights into the critical design of weakly solvated Zn^(2+) þand desolvation processes at heterointerfaces.展开更多
The pervasive adoption of 5th generation mobile communication technology propels electromagnetic wave(EW)absorbents to achieve high-level performance.The heterointerface construction is crucial to the improvement of a...The pervasive adoption of 5th generation mobile communication technology propels electromagnetic wave(EW)absorbents to achieve high-level performance.The heterointerface construction is crucial to the improvement of absorption ability.Herein,a series of ultralight composites with rational heterointerfaces(Co/ZnO@N-doped C/layer-stacked C,MSC)is fabricated by calcination with ration-al construction of sugarcane and CoZn-zeolitic imidazolate framework(ZIF).The components and structures of as-prepared composites were investigated,and their electromagnetic parameters could be adjusted by the content of CoZn-ZIFs.All composites possess excellent EW absorption performance,especially MSC-3.The optimal minimum reflection loss and effective absorption band of MSC-3 can reach−42 dB and 7.28 GHz at the thickness of only 1.6 mm with 20wt%filler loading.This excellent performance is attributed to the syner-gistic effect of dielectric loss stemming from the multiple heterointerfaces and magnetic loss induced by magnetic single Co.The sugar-cane-derived layer-stacked carbon has formed consecutive conductive networks and has further dissipated the electromagnetic energy through multiple reflection and conduction losses.Moreover,the simulated radar cross section(RCS)technology manifests that MSC-3 possesses outstanding EW attenuation capacity under realistic far-field conditions.This study provides a strategy for building efficient ab-sorbents based on biomass.展开更多
The heterointerface engineering involving different components or phases represents a desirable strategy for enhancing the sluggish kinetics of hydrogen evolution reaction(HER).However,constructing desired heterointer...The heterointerface engineering involving different components or phases represents a desirable strategy for enhancing the sluggish kinetics of hydrogen evolution reaction(HER).However,constructing desired heterointerfaces and elucidating the reaction mechanisms on the interface remains a considerable challenge.In this work,we propose a straightforward electrochemical synthesis strategy to prepare the nickel sulfide-based heterointerfaces for HER.The mechanism of electrochemical synthesis is revealed,wherein metal-thiourea species can be formed at the cathode potential and subsequently oxidized to nickel sulfides at the anode potentials.Leveraging this mechanism,a range of nickel sulfides,including NiS,Ni_(3)S_(2)/NiS,Ni/Ni_(3)S_(2)and Ni_(3)S_(2),have been successfully synthesized by tuning the potential range of cyclic voltammetry.Among these,the obtained Ni_(3)S_(2)/NiS@CC(CC:carbon cloth)exhibits the smallest overpotential of84 mV at 10 mA·cm^(-2)and high stability.Theoretical calculations further reveal that the combination of NiS and Ni_(3)S_(2)induces electron redistribution at the interface,and thus the Volmer process is effectively promoted with faster water dissociation and OH desorption kinetics.Significantly,the simplicity method coupled with a clear synthesis mechanism and outstanding HER performance highlights its promising potential for practical applications.展开更多
Superlubricity,a novel lubricity mode ascribing to moirésuperlattice(MSL),has attracted attention in ultra-precise manufacture,microelectronic devices,and national defense areas.Based on incommensurate MSL,nearly...Superlubricity,a novel lubricity mode ascribing to moirésuperlattice(MSL),has attracted attention in ultra-precise manufacture,microelectronic devices,and national defense areas.Based on incommensurate MSL,nearly zero friction can be achieved by eliminating sliding lock-in and offsetting lateral force in principle,and the theoretical foundations are still under extensive investigation.Here,the effects of MSL-induced lattice distortion onπbond and tribological performance in twist MoS_(2)/graphene and MoS_(2)/BN heterointerfaces were studied by first-principles calculations comprehensively.Various contributions of 2pz orbital electron polarization among AA-,AB-,and AC-stacking symmetry areas in different MSL were reflected by band structures to explain the sensitivity ofπbond to MSL.Theπbond perpendicular to the atomic plane depended closely on interfacial distortion,which can not only influence the local distribution of intralayer bond strength but also determine the interlayer charge redistribution.Meanwhile,the interfacial potential energy was changed with the interlayer interaction fluctuation caused by twist angle and atomic stacking modes.Through evaluating the energy barriers and lateral force,MoS_(2)/BN with a twist angle of 20.79°exhibited superlubricity.Moreover,the connection among sliding energy barriers,twist angles,and specific electronic structures has been bridged paving a path to reveal the superlubricity mechanism of two-dimensional materials withπbond.展开更多
The development of wearable multifunctional electromagnetic protective fabrics with multifunctional,low cost,and high efficiency remains a challenge.Here,inspired by the unique flower branch shape of“Thunberg’s mead...The development of wearable multifunctional electromagnetic protective fabrics with multifunctional,low cost,and high efficiency remains a challenge.Here,inspired by the unique flower branch shape of“Thunberg’s meadowsweet”in nature,a nanofibrous composite membrane with hierarchical structure was constructed.Integrating sophisticated 0D@2D@1D hierarchical structures with multiple heterointerfaces can fully unleash the multifunctional application potential of composite membrane.The targeted induction method was used to precisely regulate the formation site and morphology of the metal–organic framework precursor,and intelligently integrate multiple heterostructures to enhance dielectric polarization,which improves the impedance matching and loss mechanisms of the electromagnetic wave absorbing materials.Due to the synergistic enhancement of electrospinning-derived carbon nanofiber“stems”,MOF-derived carbon nanosheet“petals”and transition metal selenide nano-particle“stamens”,the CoxSey/NiSe@CNSs@CNFs(CNCC)composite membrane obtains a minimum reflection loss value(RL_(min))of-68.40 dB at 2.6 mm and a maximum effective absorption bandwidth(EAB)of 8.88 GHz at a thin thickness of 2.0 mm with a filling amount of only 5 wt%.In addition,the multi-component and hierarchical heterostructure endow the fibrous membrane with excellent flexibility,water resistance,thermal management,and other multifunctional properties.This work provides unique perspectives for the precise design and rational application of multifunctional fabrics.展开更多
Multiphase polymer-derived ceramics have the advantages of thermal stability and adjustable dielectric properties,which exhibit significant potential for use in high-temperature microwave absorbing materials.Herein,Co...Multiphase polymer-derived ceramics have the advantages of thermal stability and adjustable dielectric properties,which exhibit significant potential for use in high-temperature microwave absorbing materials.Herein,Co-containing polymer-derived SiCN(Co-SiCN)ceramics were successfully synthesized by the physical mixing of zeolitic imidazolate framework(ZIF)-67 and polysilazane precursors and subsequent pyrolysis.The phase and chemical compositions,microstructures,dielectric properties,electromagnetic wave absorption(EWA)performance,and mechanism of the ceramics were investigated.The results showed that the introduction of ZIF-67 promoted the in situ formation of dielectric loss phases,including SiC nanocrystals,CoSi nanocrystals,and free carbon.The phase composition can be regulated by controlling the pyrolysis temperature to achieve ideal EWA properties.The Co-SiCN ceramic pyrolyzed at 1500℃demonstrated excellent EWA performance,with a maximum effective absorption band(EAB_(max))of 3.0 GHz at an ultralow thickness of 1.05 mm and minimum reflection loss(RL_(min))of-46.4 dB at a low frequency of 6 GHz.Compared with other reported SiCN-based ceramics containing magnetic metals,the ceramics prepared in this study stand out because of their low RL and high EAB at low thicknesses.The superior microwave absorption performance of the Co-SiCN ceramics is attributed to the heterointerface polarization,and impedance matching induced by the synergistic effects of their co-existing electromagnetic transparent/absorption phases.This study provides new insights into the development of high-performance SiCNbased microwave absorbers.展开更多
Zinc-air batteries(ZABs) with high energy density and safety are promising as next-generation energy storage systems, while their applications are severely hindered by the sluggish reaction kinetic of air cathodes. De...Zinc-air batteries(ZABs) with high energy density and safety are promising as next-generation energy storage systems, while their applications are severely hindered by the sluggish reaction kinetic of air cathodes. Developing a bifunctional catalyst with high activity and durability is an effective strategy to address the above challenges. Herein, a Co_(3)O_(4)/Mn_(3)O_(4) nanohybrid with heterointerfaces is designed as advanced cathode catalyst for ZABs. Density functional theory calculations show the heterogeneous interface between Co_(3)O_(4)/Mn_(3)O_(4) can improve the dynamics of carrier transport and thus enhancing the catalytic activity and durability. The Co_(3)O_(4)/Mn_(3)O_(4) catalyst anchored on reduced graphene oxide(rGO)exhibits high oxygen reduction reaction(ORR) activity with a half-wave potential of 0.86 V, and excellent oxygen evolution reaction(OER) activity with the potential of 1.59 V at 10 mA cm^(-2) , which are comparable to the commercial noble metal catalysts. The improved ORR/OER catalytic activity is ascribed to the synergistic effect of heterointerfaces between Co_(3)O_(4) and Mn_(3)O_(4)as well as the improved conductivity and contact area of oxygen/catalysts/electrolytes three-phase interface by r GO. Furthermore, a home-made ZAB based on Co_(3)O_(4)/Mn_(3)O_(4)/r GO shows a high open circuit voltage of 1.54 V, a large power density of 194.6 mW cm^(-2) and good long-term cycling stability of nearly 400 h at 5 mA cm^(-2) , which affords a promising bifunctional oxygen catalyst for rechargeable ZABs.展开更多
The two-dimensional electron gas at SrTiO3-based heterointerfaces has received a great deal of attention in recent years owing to their potential for the exploration of emergent physics and the next generation of elec...The two-dimensional electron gas at SrTiO3-based heterointerfaces has received a great deal of attention in recent years owing to their potential for the exploration of emergent physics and the next generation of electronics. One of the most fascinating aspects in this system is that the light, as a powerful external perturbation, can modify its transport properties. Recent studies have reported that SrTiO3-based heterointerfaces exhibit the persistent photoconductivity and can be tuned by the surface and interface engineering. These researches not only reveal the intrinsic physical mechanisms in the photoresponsive process, but also highlight the ability to be used as a tool for novel all-oxide optical devices. This review mainly contraposes the studies of photoresponse at SrTiO3-based heterointerfaces.展开更多
Interface issues have consistently impeded efforts to balance a trade-off between the conductivity functionality and mechanical properties of Cu-matrix composites.Combining first-principles simulations,this study addr...Interface issues have consistently impeded efforts to balance a trade-off between the conductivity functionality and mechanical properties of Cu-matrix composites.Combining first-principles simulations,this study addresses this challenge by preparing a new Cumatrix composite reinforced with MXene,Cu/Ag@MXene composite block(CuAM-CB),which improves the compatibility between metallic Cu and nonmetallic MXene facilitated by Ag modification anchored in situ onto MXene nanosheets,thus realizing element-coupled reinforcement of Ag at the Cu/MXene heterointerfaces.Benefiting from the strong interaction between Ag and C atoms from in situ self-reduction,as well as the excellent compatibility between Ag and Cu atoms(both IB group metals),Ag atoms act as a mediator for the electron transport and mechanical connection at the Cu/MXene heterointerfaces,enabling CuAM-CB to achieve integrated high conductivity functionality(up to 95%IACS)and strong mechanical properties(with a strength-plasticity product of∼18 GPa%).展开更多
Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,how...Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.展开更多
The synthesis of carbon supporter/nanoscale high-entropy alloys(HEAs)electromagnetic response composites by carbothermal shock method has been identified as an advanced strategy for the collaborative competition engin...The synthesis of carbon supporter/nanoscale high-entropy alloys(HEAs)electromagnetic response composites by carbothermal shock method has been identified as an advanced strategy for the collaborative competition engineering of conductive/dielectric genes.Electron migration modes within HEAs as manipulated by the electronegativity,valence electron configurations and molar proportions of constituent elements determine the steady state and efficiency of equivalent dipoles.Herein,enlightened by skin-like effect,a reformative carbothermal shock method using carbonized cellulose paper(CCP)as carbon supporter is used to preserve the oxygencontaining functional groups(O·)of carbonized cellulose fibers(CCF).Nucleation of HEAs and construction of emblematic shell-core CCF/HEAs heterointerfaces are inextricably linked to carbon metabolism induced by O·.Meanwhile,the electron migration mode of switchable electronrich sites promotes the orientation polarization of anisotropic equivalent dipoles.By virtue of the reinforcement strategy,CCP/HEAs composite prepared by 35%molar ratio of Mn element(CCP/HEAs-Mn_(2.15))achieves efficient electromagnetic wave(EMW)absorption of−51.35 dB at an ultra-thin thickness of 1.03 mm.The mechanisms of the resulting dielectric properties of HEAs-based EMW absorbing materials are elucidated by combining theoretical calculations with experimental characterizations,which provide theoretical bases and feasible strategies for the simulation and practical application of electromagnetic functional devices(e.g.,ultra-wideband bandpass filter).展开更多
Currently,although some progress has been made in infancy-stage rocking-chair aqueous zinc-ion batteries(AZIBs),more discussions have focused only on the different electrochemical performances displayed by different m...Currently,although some progress has been made in infancy-stage rocking-chair aqueous zinc-ion batteries(AZIBs),more discussions have focused only on the different electrochemical performances displayed by different material types rather than the intrinsic ion transport migration electrochemistry.Herein,we for the first time delve into the mechanism of tailoring the solvation sheath and desolvation processes at the electrode/electrolyte interfaces to enhance the structural stabilities in the deep discharge states.In this work,the TiO_(2)front interfaces are induced on electrochemically active but unstable TiSe_(2)host materials to construct unique TiO_(2)/TiSe_(2)-C heterointerfaces.According to X-ray absorption near edge structure(XANES),differential electrochemical mass spectrometry(DEMS),and electrochemical quartz crystal microbalance(EQCM),the intercalated species are transformed from[Zn(H_(2)O)_(6)]^(2+)to[Zn(H_(2)O)_(2)]^(2+)due to the built-in electric fields(BEFs)effects,further accelerating the ion transfer kinetics.Furthermore,owing to the absence of high-energy desolvation solvents released from desolvation processes,hydrogen evolution reaction(HER)energy barriers,Ti-Se bond strength,and structural stabilities are significantly improved,and the initial CE and HER overpotentials of the TiO_(2)/TiSe_(2)-C heterointerfaces increased from 13.76%to 84.7%,and from 1.04 to 1.30 V,respectively,and the H2 precipitation current density even at-1.3 V decreased by 73.2%.This work provides valuable insights into the complex interface electrochemical mechanism of tailoring the solvation sheath and desolvation processes toward rocking-chair zinc-ion batteries.展开更多
Bismuth-based materials are prevalent catalysts for CO_(2)electroreduction to formate,enduring high hydrogen evolution reactions and inadequate activity and stability.Herein,we reveal that in-situ electrochemical tran...Bismuth-based materials are prevalent catalysts for CO_(2)electroreduction to formate,enduring high hydrogen evolution reactions and inadequate activity and stability.Herein,we reveal that in-situ electrochemical transformation of Cu_(2)BiS_(x)solid solution into Bi/Cu_(x)S_(y)heterointerfaces,which can stabilize the intermediates and achieve highly selective and consistent CO_(2)electroreduction.It shows over 85%Faraday efficiency(FE)of formate with a potential window of−0.8 to−1.2 VRHE(RHE:reversible hydrogen electrode)and a stability above 90%over 27 h in H-type cell at−0.9 VRHE.It maintains more than 85%of FEformate at the current density of−25 to−200 mA·cm^(−2),has stability of about 80%of FEformate at least 10 h at−150 mA·cm^(−2)in flow cell.In-situ Fourier transform infrared(FT-IR)spectroscopy measurement confirms that the preferred route of catalytic reaction is to generate *CO_(2)^(−) and *OCHO intermediates.The density functional theory(DFT)calculations illustrate that heterointerfaces facilitate the prior process of CO_(2)to HCOOH through *OCHO by additional Bi hybrid orbitals.This study is expected to open up a new idea for the design of CO_(2)electroreduction catalyst.展开更多
Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3...Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.展开更多
Developing electrocatalysts to inhibit polysulfide shuttling and expedite sulfur species conversion is vital for the evolution of Lithium-sulfur(Li-S)batteries.This work provides a facile strategy to design an intimat...Developing electrocatalysts to inhibit polysulfide shuttling and expedite sulfur species conversion is vital for the evolution of Lithium-sulfur(Li-S)batteries.This work provides a facile strategy to design an intimate heterostructure of MIL-88A@CdS as a sulfur electrocatalyst combining high sulfur adsorption and accelerated polysulfide conversion.The MIL-88A can give a region of high-ordered polysulfide adsorption,whereas the CdS is an effective nanoreactor for the sulfur reduction reaction(SRR).Notedly,the significant size difference between MIL-88A and CdS enables the unique heterostructure interactions.The largesize MIL-88A ensures a uniform distribution of CdS nanoparticles as a substrate.This configuration facilitates control of the initial polysulfide adsorption position relative to its final deposition site as lithium sulfide.The heterostructure also demonstrates rapid transport and efficient conversion of lithium polysulfides.Consequently,the Li-S battery with MIL-88A@CdS heterostructure modified separator delivers exceptional performance,achieving an areal capacity exceeding 6 mAh cm^(−2),an excellent rate capability of 980 mAh g^(−1) at 5 C,and notable cycling stability in a 2 Ah pouch cell over 100 cycles.This work is significant for elucidating the relationship between heterostructure and electrocatalytic performance,providing great insights for material design aimed at highly efficient future electrocatalysts in practical applications.展开更多
Constructing a valid heterointerface with a built-in electric field is an effective strategy for designing energy storage anodes with exceptional efficiency for potassium-ion batteries(PIBs)and sodium-ion batteries(SI...Constructing a valid heterointerface with a built-in electric field is an effective strategy for designing energy storage anodes with exceptional efficiency for potassium-ion batteries(PIBs)and sodium-ion batteries(SIBs).In this study,WSe_(2)/MoSe_(2)nanosheets with a better-matched and stable heterojunction interface were uniformly embedded in carbon nanofiber frameworks(WSe_(2)/MoSe_(2)/CNFs).The ion/electron transfer kinetics were facilitated by heterointerfaces with an enlarged effective utilization range.Meanwhile,the heterointerface directed electron transfer from MoSe_(2)to WSe_(2)and had significant potassium adsorption capability.The ultra-high pseudocapacitance contribution originating from the heterostructure and morphological features of the WSe_(2)/MoSe_(2)nanosheets contributed to enhancing high-rate energy storage.Moreover,in situ X-ray diffraction and ex situ X-ray photoelectron spectroscopy revealed the potassification/depotassification behavior of the WSe_(2)/MoSe_(2)/CNFs during the conversion reaction.Consequently,after 500 cycles at 5 A·g^(-1),the WSe_(2)/MoSe_(2)/CNF anode demonstrated an outstanding long-term cycling performance of 125.6 mAh·g^(-1)for PIBs.While serving as a SIB electrode,it exhibited an exceptional rate capability of 243.5 mAh·g^(-1)at 20 A·g^(-1).With the goal of developing high-performance PIB/SIB electrode materials,the proposed strategy,based on heterointerface adaptation engineering,is promising.展开更多
Sustainable H_(2) production based on hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) has attracted wide attention due to minimal energy consumption compared to overall water electrolysis.The...Sustainable H_(2) production based on hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) has attracted wide attention due to minimal energy consumption compared to overall water electrolysis.The present study focuses on the design and construction of heterostructured CoPB@NiFe-OH applied as efficient bifunctional catalysts to sustainably produce hydrogen and remove hydrazine in alkaline media.Impressively,CoPB@NiFe-OH heterointerface exhibits an HzOR potential of-135 mV at the current density of 10 mA cm^(2) when the P to B atom ratio was 0.2,simultaneously an HER potential of-32 mV toward HER when the atom ratio of P and B was 0.5.Thus,hydrogen production without an outer voltage accompanied by a small current density output of 25 mA cm^(2) is achieved,surpassing most reported catalysts.In addition,DFT calculations demonstrate the Co sites in CoPB upgrades H*adsorption,while the Ni sites in NiFe-OH optimizes the adsorption energy of N_(2)H_(4)*due to electron transfer from CoPB to NiFe-OH at the heterointerface,ultimately leading to exceptional performance in hydrazine-assistant water electrolysis via HER coupled with HzOR.展开更多
基金supported by the Beijing Natural Science Foundation(Grant No.JQ24002)the National Key Basic Research Program of China(Grant No.2020YFA0309100)+3 种基金the National Natural Science Foundation of China(Grant Nos.U22A20263,52250308,12304158,12325401,12274069,12404102,and 12474096)the Chinese Academy of Sciences(CAS)Project for Young Scientists in Basic Research(Grant No.YSBR-084)the CAS Youth Interdisciplinary Team,the Guangdong Basic and Applied Basic Research Foundation(Grant No.2022B1515120014)the Guangdong-Hong Kong-Macao Joint Laboratory for Neutron Scattering Science and Technology,and the International Young Scientist Fellowship of Institute of Physics,CAS.
文摘Heterointerfaces have been pivotal in unveiling extraordinary interfacial properties and enabling multifunctional material platforms.Despite extensive research on all-oxide interfaces,heterointerfaces between different material classes,such as oxides and nitrides,remain underexplored.Here we present the fabrication of atomically sharp heterointerfaces between antiperovskite Ni_(3)InN and perovskite SrVO_(3).Leveraging layer-resolved scanning transmission electron microscopy and electron energy loss spectroscopy,we identified pronounced charge transfer across the well-ordered interface.First-principles calculations confirmed our experimental observations and further predicted an emergent magnetic moment within the Ni_(3)InN layer due to the charge transfer.These findings pave the way for novel electronic and spintronic applications by enabling tunable interfacial properties in nitride/oxide systems.
基金financially supported by the National Natural Science Foundation of China(52373271)Science,Technology and Innovation Commission of Shenzhen Municipality under Grant(KCXFZ20201221173004012)+1 种基金National Key Research and Development Program of Shaanxi Province(No.2023-YBNY-271)Open Testing Foundation of the Analytical&Testing Center of Northwestern Polytechnical University(2023T019).
文摘Gradient magnetic heterointerfaces have injected infinite vitality in optimizing impedance matching,adjusting dielectric/magnetic resonance and promoting electromagnetic(EM)wave absorption,but still exist a significant challenging in regulating local phase evolution.Herein,accordion-shaped Co/Co_(3)O_(4)@N-doped carbon nanosheets(Co/Co_(3)O_(4)@NC)with gradient magnetic heterointerfaces have been fabricated via the cooperative high-temperature carbonization and lowtemperature oxidation process.The results indicate that the surface epitaxial growth of crystal Co_(3)O_(4) domains on local Co nanoparticles realizes the adjustment of magnetic-heteroatomic components,which are beneficial for optimizing impedance matching and interfacial polarization.Moreover,gradient magnetic heterointerfaces simultaneously realize magnetic coupling,and long-range magnetic diffraction.Specifically,the synthesized Co/Co_(3)O_(4)@NC absorbents display the strong electromagnetic wave attenuation capability of−53.5 dB at a thickness of 3.0 mm with an effective absorption bandwidth of 5.36 GHz,both are superior to those of single magnetic domains embedded in carbon matrix.This design concept provides us an inspiration in optimizing interfacial polarization,regulating magnetic coupling and promoting electromagnetic wave absorption.
基金supported by the National Natural Science Foundation of China(No.22269010)Jiangxi Provincial Natural Science Foundation(No.20224BAB214021)the Opening Project of National Engineering Research Center for Domestic&Building Ceramics(No.GXZX2302).
文摘The existence of multiple vacancies leads to significant changes in the local atomic structure,which can regulate the electronic structure of the surface and form unsaturated coordination geometries.However,the current methods employed to generate multiple vacancies in two-dimensional(2D)layered double hydroxide(LDH)materials are still difficult to achieve to some extent and are primarily limited to monolayer LDH structures.Here,we present an improved method to synthesize NiMoP/Ni_(2)P catalysts with a sponge-like porous structure.Firstly,NiO with dual defects was constructed by subjecting NiMo-LDH/Ni to air calcination.Subsequently,we performed phosphorization treatment and introduced multiple Ni vacancies and O vacancies as defect sites to tune the edge and substrate surfaces of LDH.At the same time,the electronic structure was tuned by adding P heteroatoms.The synergistic effect of porous structure,heterogeneous interfaces,vacancies,doping defects,and amorphous states can greatly enhance the electron transfer effect inside the catalysts,which significantly improves the catalytic ability of the oxygen evolution reaction(OER).Therefore,the overpotential for the oxygen evolution reaction of NiMoP/Ni_(2)P heterointerfaces reaches 270 mV at a current density of 10 mA·cm^(-2)under alkaline conditions,with the catalysts capable of sustaining high current densities even after the durability testing for 35 h.
基金financially supported by the National Natural Science Foundation of China(51977097).
文摘Solvated zinc ions are prone to undergo desolvation at the electrode/electrolyte interfaces,and unstable H_(2)O molecules within the solvated sheaths tend to trigger hydrogen evolution reaction(HER),further accelerating interfaces decay.Herein,we propose for the first time a novel strategy to enhance the interfacial stabilities by insitu dynamic reconstruction of weakly solvated Zn2þduring the desolvation processes at heterointerfaces.Theoretical calculations indicate that,due to built-in electric field effects(BEFs),the plating/stripping mechanism shifts from[Zn(H_(2)O)_(6)]_(2)þto[Zn(H_(2)O)_(5)(SO_(4))^(2-)]_(2)þwithout additional electrolyte additives,reducing the solvation ability of H_(2)O,enhancing the competitive coordination of SO_(4)^(2-),essentially eliminating the undesirable side effects of anodes.Hence,symmetric cells can operate stably for 3000 h(51.7-times increase in cycle life),and the full cells can operate stably for 5000 cycles(51.5-times increase in cycle life).This study provides valuable insights into the critical design of weakly solvated Zn^(2+) þand desolvation processes at heterointerfaces.
基金supported by the National-Natural Science Foundation of China(Nos.52302362,52377026,and 52301192)Doctorial Foundation of Henan University of Technology,China(Nos.2021BS030 and 2020BS030)+3 种基金Key Scientific and Technological Research Projects in Henan Province,China(Nos.222102240091 and 232102240038)Natural Science Foundation from the Department of Science and Technology of Henan Province,China(No.232300420309)Taishan Scholars and Young Experts Program of Shandong Province,China(No.tsqn202103057)“Sanqin Scholars”Innovation Teams Project of Shaanxi Province,China(Clean Energy Materials and High-Performance Devices Innovation Team of Shaanxi Dongling Smelting Co.,Ltd.).
文摘The pervasive adoption of 5th generation mobile communication technology propels electromagnetic wave(EW)absorbents to achieve high-level performance.The heterointerface construction is crucial to the improvement of absorption ability.Herein,a series of ultralight composites with rational heterointerfaces(Co/ZnO@N-doped C/layer-stacked C,MSC)is fabricated by calcination with ration-al construction of sugarcane and CoZn-zeolitic imidazolate framework(ZIF).The components and structures of as-prepared composites were investigated,and their electromagnetic parameters could be adjusted by the content of CoZn-ZIFs.All composites possess excellent EW absorption performance,especially MSC-3.The optimal minimum reflection loss and effective absorption band of MSC-3 can reach−42 dB and 7.28 GHz at the thickness of only 1.6 mm with 20wt%filler loading.This excellent performance is attributed to the syner-gistic effect of dielectric loss stemming from the multiple heterointerfaces and magnetic loss induced by magnetic single Co.The sugar-cane-derived layer-stacked carbon has formed consecutive conductive networks and has further dissipated the electromagnetic energy through multiple reflection and conduction losses.Moreover,the simulated radar cross section(RCS)technology manifests that MSC-3 possesses outstanding EW attenuation capacity under realistic far-field conditions.This study provides a strategy for building efficient ab-sorbents based on biomass.
基金financially supported by the National Natural Science Foundation of China(No.22202042)Guangdong Basic and Applied Basic Research Foundation(No.2022A1515140012)Yunnan Fundamental Research Projects(grant No.202401CF070036)。
文摘The heterointerface engineering involving different components or phases represents a desirable strategy for enhancing the sluggish kinetics of hydrogen evolution reaction(HER).However,constructing desired heterointerfaces and elucidating the reaction mechanisms on the interface remains a considerable challenge.In this work,we propose a straightforward electrochemical synthesis strategy to prepare the nickel sulfide-based heterointerfaces for HER.The mechanism of electrochemical synthesis is revealed,wherein metal-thiourea species can be formed at the cathode potential and subsequently oxidized to nickel sulfides at the anode potentials.Leveraging this mechanism,a range of nickel sulfides,including NiS,Ni_(3)S_(2)/NiS,Ni/Ni_(3)S_(2)and Ni_(3)S_(2),have been successfully synthesized by tuning the potential range of cyclic voltammetry.Among these,the obtained Ni_(3)S_(2)/NiS@CC(CC:carbon cloth)exhibits the smallest overpotential of84 mV at 10 mA·cm^(-2)and high stability.Theoretical calculations further reveal that the combination of NiS and Ni_(3)S_(2)induces electron redistribution at the interface,and thus the Volmer process is effectively promoted with faster water dissociation and OH desorption kinetics.Significantly,the simplicity method coupled with a clear synthesis mechanism and outstanding HER performance highlights its promising potential for practical applications.
基金financially supported by the National Key Re-search and Development Program of China(Nos.2018YFB0703801 and 2018YFB0703802)the Foundation for Doctor Dissertation of Northwestern Polytechnical University(No.CX2021064)。
文摘Superlubricity,a novel lubricity mode ascribing to moirésuperlattice(MSL),has attracted attention in ultra-precise manufacture,microelectronic devices,and national defense areas.Based on incommensurate MSL,nearly zero friction can be achieved by eliminating sliding lock-in and offsetting lateral force in principle,and the theoretical foundations are still under extensive investigation.Here,the effects of MSL-induced lattice distortion onπbond and tribological performance in twist MoS_(2)/graphene and MoS_(2)/BN heterointerfaces were studied by first-principles calculations comprehensively.Various contributions of 2pz orbital electron polarization among AA-,AB-,and AC-stacking symmetry areas in different MSL were reflected by band structures to explain the sensitivity ofπbond to MSL.Theπbond perpendicular to the atomic plane depended closely on interfacial distortion,which can not only influence the local distribution of intralayer bond strength but also determine the interlayer charge redistribution.Meanwhile,the interfacial potential energy was changed with the interlayer interaction fluctuation caused by twist angle and atomic stacking modes.Through evaluating the energy barriers and lateral force,MoS_(2)/BN with a twist angle of 20.79°exhibited superlubricity.Moreover,the connection among sliding energy barriers,twist angles,and specific electronic structures has been bridged paving a path to reveal the superlubricity mechanism of two-dimensional materials withπbond.
基金supported by the National Natural Science Foundation of China(No.51407134,No.52002196)Natural Science Foundation of Shandong Province(No.ZR2019YQ24,No.ZR2020QF084)+2 种基金Taishan Scholars and Young Experts Program of Shandong Province(No.tsqn202103057)the Qingchuang Talents Induction Program of Shandong Higher Education Institution(Research and Innovation Team of Structural-Functional Polymer Composites)Special Financial of Shandong Province(Structural Design of Highefficiency Electromagnetic Wave-absorbing Composite Materials and Construction of Shandong Provincial Talent Teams(No.37000022P990304116449)).
文摘The development of wearable multifunctional electromagnetic protective fabrics with multifunctional,low cost,and high efficiency remains a challenge.Here,inspired by the unique flower branch shape of“Thunberg’s meadowsweet”in nature,a nanofibrous composite membrane with hierarchical structure was constructed.Integrating sophisticated 0D@2D@1D hierarchical structures with multiple heterointerfaces can fully unleash the multifunctional application potential of composite membrane.The targeted induction method was used to precisely regulate the formation site and morphology of the metal–organic framework precursor,and intelligently integrate multiple heterostructures to enhance dielectric polarization,which improves the impedance matching and loss mechanisms of the electromagnetic wave absorbing materials.Due to the synergistic enhancement of electrospinning-derived carbon nanofiber“stems”,MOF-derived carbon nanosheet“petals”and transition metal selenide nano-particle“stamens”,the CoxSey/NiSe@CNSs@CNFs(CNCC)composite membrane obtains a minimum reflection loss value(RL_(min))of-68.40 dB at 2.6 mm and a maximum effective absorption bandwidth(EAB)of 8.88 GHz at a thin thickness of 2.0 mm with a filling amount of only 5 wt%.In addition,the multi-component and hierarchical heterostructure endow the fibrous membrane with excellent flexibility,water resistance,thermal management,and other multifunctional properties.This work provides unique perspectives for the precise design and rational application of multifunctional fabrics.
基金financially supported by the National Natural Science Foundation of China(Nos.62071239,52102361)the Natural Science Foundation of Jiangsu Province(No.BK20200827)+1 种基金the National Key Laboratory on Electromagnetic Environmental Effects and Electro-optical Engineering(No.JCKYS2022LD2)the Startup Foundation for Introducing Talent of NUIST(No.2020r025)。
文摘Multiphase polymer-derived ceramics have the advantages of thermal stability and adjustable dielectric properties,which exhibit significant potential for use in high-temperature microwave absorbing materials.Herein,Co-containing polymer-derived SiCN(Co-SiCN)ceramics were successfully synthesized by the physical mixing of zeolitic imidazolate framework(ZIF)-67 and polysilazane precursors and subsequent pyrolysis.The phase and chemical compositions,microstructures,dielectric properties,electromagnetic wave absorption(EWA)performance,and mechanism of the ceramics were investigated.The results showed that the introduction of ZIF-67 promoted the in situ formation of dielectric loss phases,including SiC nanocrystals,CoSi nanocrystals,and free carbon.The phase composition can be regulated by controlling the pyrolysis temperature to achieve ideal EWA properties.The Co-SiCN ceramic pyrolyzed at 1500℃demonstrated excellent EWA performance,with a maximum effective absorption band(EAB_(max))of 3.0 GHz at an ultralow thickness of 1.05 mm and minimum reflection loss(RL_(min))of-46.4 dB at a low frequency of 6 GHz.Compared with other reported SiCN-based ceramics containing magnetic metals,the ceramics prepared in this study stand out because of their low RL and high EAB at low thicknesses.The superior microwave absorption performance of the Co-SiCN ceramics is attributed to the heterointerface polarization,and impedance matching induced by the synergistic effects of their co-existing electromagnetic transparent/absorption phases.This study provides new insights into the development of high-performance SiCNbased microwave absorbers.
基金support from the National Key Research and Development Program of China (2019YFA0705700)the National Natural Science Foundation of China (52072205)+1 种基金the start-up funds of Tsinghua Shenzhen International Graduate Schoosupported by the China Postdoctoral Science Foundation(2020M680542)。
文摘Zinc-air batteries(ZABs) with high energy density and safety are promising as next-generation energy storage systems, while their applications are severely hindered by the sluggish reaction kinetic of air cathodes. Developing a bifunctional catalyst with high activity and durability is an effective strategy to address the above challenges. Herein, a Co_(3)O_(4)/Mn_(3)O_(4) nanohybrid with heterointerfaces is designed as advanced cathode catalyst for ZABs. Density functional theory calculations show the heterogeneous interface between Co_(3)O_(4)/Mn_(3)O_(4) can improve the dynamics of carrier transport and thus enhancing the catalytic activity and durability. The Co_(3)O_(4)/Mn_(3)O_(4) catalyst anchored on reduced graphene oxide(rGO)exhibits high oxygen reduction reaction(ORR) activity with a half-wave potential of 0.86 V, and excellent oxygen evolution reaction(OER) activity with the potential of 1.59 V at 10 mA cm^(-2) , which are comparable to the commercial noble metal catalysts. The improved ORR/OER catalytic activity is ascribed to the synergistic effect of heterointerfaces between Co_(3)O_(4) and Mn_(3)O_(4)as well as the improved conductivity and contact area of oxygen/catalysts/electrolytes three-phase interface by r GO. Furthermore, a home-made ZAB based on Co_(3)O_(4)/Mn_(3)O_(4)/r GO shows a high open circuit voltage of 1.54 V, a large power density of 194.6 mW cm^(-2) and good long-term cycling stability of nearly 400 h at 5 mA cm^(-2) , which affords a promising bifunctional oxygen catalyst for rechargeable ZABs.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.51572222 and 11604265)Innovation Foundation for Doctor Dissertation of Northwestern Polytechnical University,China(Grant No.CX201836)
文摘The two-dimensional electron gas at SrTiO3-based heterointerfaces has received a great deal of attention in recent years owing to their potential for the exploration of emergent physics and the next generation of electronics. One of the most fascinating aspects in this system is that the light, as a powerful external perturbation, can modify its transport properties. Recent studies have reported that SrTiO3-based heterointerfaces exhibit the persistent photoconductivity and can be tuned by the surface and interface engineering. These researches not only reveal the intrinsic physical mechanisms in the photoresponsive process, but also highlight the ability to be used as a tool for novel all-oxide optical devices. This review mainly contraposes the studies of photoresponse at SrTiO3-based heterointerfaces.
基金financially supported by the Central government guides local science and technology development(CN)(No.[2019]4011)the Construction project of anti-fatigue manufacturing technology innovation ability of key components in aerospace(CN)(No.Qian financial workers[2022]92)+3 种基金the Construction of collaborative innovation platform for fatigue resistance manufacturing technology and quality reliability of key components(CN)(No.2016034)the National natural science foundation of china(CN)(No.12105059)the Guizhou provincial science and technology projects(CN)(No.ZK[2022]097)the Talented program of guizhou university(CN)(No.20210032).
文摘Interface issues have consistently impeded efforts to balance a trade-off between the conductivity functionality and mechanical properties of Cu-matrix composites.Combining first-principles simulations,this study addresses this challenge by preparing a new Cumatrix composite reinforced with MXene,Cu/Ag@MXene composite block(CuAM-CB),which improves the compatibility between metallic Cu and nonmetallic MXene facilitated by Ag modification anchored in situ onto MXene nanosheets,thus realizing element-coupled reinforcement of Ag at the Cu/MXene heterointerfaces.Benefiting from the strong interaction between Ag and C atoms from in situ self-reduction,as well as the excellent compatibility between Ag and Cu atoms(both IB group metals),Ag atoms act as a mediator for the electron transport and mechanical connection at the Cu/MXene heterointerfaces,enabling CuAM-CB to achieve integrated high conductivity functionality(up to 95%IACS)and strong mechanical properties(with a strength-plasticity product of∼18 GPa%).
基金financially supported by the National Natural Science Foundation of China(Grants nos.62201411,62371378,22205168,52302150 and 62304171)the China Postdoctoral Science Foundation(2022M722500)+1 种基金the Fundamental Research Funds for the Central Universities(Grants nos.ZYTS2308 and 20103237929)Startup Foundation of Xidian University(10251220001).
文摘Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.
基金Financial support from the National Natural Science Foundation of China(52372289,52102368,52231007,12327804,T2321003,22088101,22178037 and U22A20424)Regional Joint Fund for Basic Research and Applied Basic Research of Guangdong Province(No.2020A1515110905)+1 种基金Guangdong Special Fund for key Areas(20237DZX3042)Shenzhen Stable Support Project,Liaoning Revitalization Talents Program(XLYC2002114)are highly appreciated.
文摘The synthesis of carbon supporter/nanoscale high-entropy alloys(HEAs)electromagnetic response composites by carbothermal shock method has been identified as an advanced strategy for the collaborative competition engineering of conductive/dielectric genes.Electron migration modes within HEAs as manipulated by the electronegativity,valence electron configurations and molar proportions of constituent elements determine the steady state and efficiency of equivalent dipoles.Herein,enlightened by skin-like effect,a reformative carbothermal shock method using carbonized cellulose paper(CCP)as carbon supporter is used to preserve the oxygencontaining functional groups(O·)of carbonized cellulose fibers(CCF).Nucleation of HEAs and construction of emblematic shell-core CCF/HEAs heterointerfaces are inextricably linked to carbon metabolism induced by O·.Meanwhile,the electron migration mode of switchable electronrich sites promotes the orientation polarization of anisotropic equivalent dipoles.By virtue of the reinforcement strategy,CCP/HEAs composite prepared by 35%molar ratio of Mn element(CCP/HEAs-Mn_(2.15))achieves efficient electromagnetic wave(EMW)absorption of−51.35 dB at an ultra-thin thickness of 1.03 mm.The mechanisms of the resulting dielectric properties of HEAs-based EMW absorbing materials are elucidated by combining theoretical calculations with experimental characterizations,which provide theoretical bases and feasible strategies for the simulation and practical application of electromagnetic functional devices(e.g.,ultra-wideband bandpass filter).
基金supported by the National Natural Science Foundation of China(51977097).
文摘Currently,although some progress has been made in infancy-stage rocking-chair aqueous zinc-ion batteries(AZIBs),more discussions have focused only on the different electrochemical performances displayed by different material types rather than the intrinsic ion transport migration electrochemistry.Herein,we for the first time delve into the mechanism of tailoring the solvation sheath and desolvation processes at the electrode/electrolyte interfaces to enhance the structural stabilities in the deep discharge states.In this work,the TiO_(2)front interfaces are induced on electrochemically active but unstable TiSe_(2)host materials to construct unique TiO_(2)/TiSe_(2)-C heterointerfaces.According to X-ray absorption near edge structure(XANES),differential electrochemical mass spectrometry(DEMS),and electrochemical quartz crystal microbalance(EQCM),the intercalated species are transformed from[Zn(H_(2)O)_(6)]^(2+)to[Zn(H_(2)O)_(2)]^(2+)due to the built-in electric fields(BEFs)effects,further accelerating the ion transfer kinetics.Furthermore,owing to the absence of high-energy desolvation solvents released from desolvation processes,hydrogen evolution reaction(HER)energy barriers,Ti-Se bond strength,and structural stabilities are significantly improved,and the initial CE and HER overpotentials of the TiO_(2)/TiSe_(2)-C heterointerfaces increased from 13.76%to 84.7%,and from 1.04 to 1.30 V,respectively,and the H2 precipitation current density even at-1.3 V decreased by 73.2%.This work provides valuable insights into the complex interface electrochemical mechanism of tailoring the solvation sheath and desolvation processes toward rocking-chair zinc-ion batteries.
基金the National Natural Science Foundation of China(Nos.21871005 and 22171005)the University Synergy Innovation Program of Anhui Province(Nos.GXXT-2020-005,GXXT-2021-012,and GXXT-2021-013).
文摘Bismuth-based materials are prevalent catalysts for CO_(2)electroreduction to formate,enduring high hydrogen evolution reactions and inadequate activity and stability.Herein,we reveal that in-situ electrochemical transformation of Cu_(2)BiS_(x)solid solution into Bi/Cu_(x)S_(y)heterointerfaces,which can stabilize the intermediates and achieve highly selective and consistent CO_(2)electroreduction.It shows over 85%Faraday efficiency(FE)of formate with a potential window of−0.8 to−1.2 VRHE(RHE:reversible hydrogen electrode)and a stability above 90%over 27 h in H-type cell at−0.9 VRHE.It maintains more than 85%of FEformate at the current density of−25 to−200 mA·cm^(−2),has stability of about 80%of FEformate at least 10 h at−150 mA·cm^(−2)in flow cell.In-situ Fourier transform infrared(FT-IR)spectroscopy measurement confirms that the preferred route of catalytic reaction is to generate *CO_(2)^(−) and *OCHO intermediates.The density functional theory(DFT)calculations illustrate that heterointerfaces facilitate the prior process of CO_(2)to HCOOH through *OCHO by additional Bi hybrid orbitals.This study is expected to open up a new idea for the design of CO_(2)electroreduction catalyst.
基金Research Institute for Smart Energy(CDB2)the grant from the Research Institute for Advanced Manufacturing(CD8Z)+4 种基金the grant from the Carbon Neutrality Funding Scheme(WZ2R)at The Hong Kong Polytechnic Universitysupport from the Hong Kong Polytechnic University(CD9B,CDBZ and WZ4Q)the National Natural Science Foundation of China(22205187)Shenzhen Municipal Science and Technology Innovation Commission(JCYJ20230807140402006)Start-up Foundation for Introducing Talent of NUIST and Natural Science Foundation of Jiangsu Province of China(BK20230426).
文摘Catalyst–support interaction plays a crucial role in improving the catalytic activity of oxygen evolution reaction(OER).Here we modulate the catalyst–support interaction in polyaniline-supported Ni_(3)Fe oxide(Ni_(3)Fe oxide/PANI)with a robust hetero-interface,which significantly improves oxygen evolution activities with an overpotential of 270 mV at 10 mA cm^(-2)and specific activity of 2.08 mA cm_(ECSA)^(-2)at overpotential of 300 mV,3.84-fold that of Ni_(3)Fe oxide.It is revealed that the catalyst–support interaction between Ni_(3)Fe oxide and PANI support enhances the Ni–O covalency via the interfacial Ni–N bond,thus promoting the charge and mass transfer on Ni_(3)Fe oxide.Considering the excellent activity and stability,rechargeable Zn-air batteries with optimum Ni_(3)Fe oxide/PANI are assembled,delivering a low charge voltage of 1.95 V to cycle for 400 h at 10 mA cm^(-2).The regulation of the effect of catalyst–support interaction on catalytic activity provides new possibilities for the future design of highly efficient OER catalysts.
基金supported by the Natural Science Foundation of China(22309179)the Natural Science Foundation of China(12404049)+4 种基金Natural Science Foundation of Ningxia(2023AAC01003)Guangdong Basic and Applied Basic Research Foundation(2021A1515110156,2022A1515010724,2023A1515110521,2023B1515120095,2024A1515011260)Science and Technology Program of Guangzhou(No.2019050001)the Outstanding Youth Project of Guangdong Natural Science Foundation(2021B1515020051)Dalian Revitalization Talents Program(No.2022RG01).
文摘Developing electrocatalysts to inhibit polysulfide shuttling and expedite sulfur species conversion is vital for the evolution of Lithium-sulfur(Li-S)batteries.This work provides a facile strategy to design an intimate heterostructure of MIL-88A@CdS as a sulfur electrocatalyst combining high sulfur adsorption and accelerated polysulfide conversion.The MIL-88A can give a region of high-ordered polysulfide adsorption,whereas the CdS is an effective nanoreactor for the sulfur reduction reaction(SRR).Notedly,the significant size difference between MIL-88A and CdS enables the unique heterostructure interactions.The largesize MIL-88A ensures a uniform distribution of CdS nanoparticles as a substrate.This configuration facilitates control of the initial polysulfide adsorption position relative to its final deposition site as lithium sulfide.The heterostructure also demonstrates rapid transport and efficient conversion of lithium polysulfides.Consequently,the Li-S battery with MIL-88A@CdS heterostructure modified separator delivers exceptional performance,achieving an areal capacity exceeding 6 mAh cm^(−2),an excellent rate capability of 980 mAh g^(−1) at 5 C,and notable cycling stability in a 2 Ah pouch cell over 100 cycles.This work is significant for elucidating the relationship between heterostructure and electrocatalytic performance,providing great insights for material design aimed at highly efficient future electrocatalysts in practical applications.
基金supported by the National Natural Science Foundation of China(No.22201098)the Natural Science Foundation of Shandong Province(Nos.ZR2021QB005 and ZR2021MB008)Jinan City“New University 20”Project(No.202228113).
文摘Constructing a valid heterointerface with a built-in electric field is an effective strategy for designing energy storage anodes with exceptional efficiency for potassium-ion batteries(PIBs)and sodium-ion batteries(SIBs).In this study,WSe_(2)/MoSe_(2)nanosheets with a better-matched and stable heterojunction interface were uniformly embedded in carbon nanofiber frameworks(WSe_(2)/MoSe_(2)/CNFs).The ion/electron transfer kinetics were facilitated by heterointerfaces with an enlarged effective utilization range.Meanwhile,the heterointerface directed electron transfer from MoSe_(2)to WSe_(2)and had significant potassium adsorption capability.The ultra-high pseudocapacitance contribution originating from the heterostructure and morphological features of the WSe_(2)/MoSe_(2)nanosheets contributed to enhancing high-rate energy storage.Moreover,in situ X-ray diffraction and ex situ X-ray photoelectron spectroscopy revealed the potassification/depotassification behavior of the WSe_(2)/MoSe_(2)/CNFs during the conversion reaction.Consequently,after 500 cycles at 5 A·g^(-1),the WSe_(2)/MoSe_(2)/CNF anode demonstrated an outstanding long-term cycling performance of 125.6 mAh·g^(-1)for PIBs.While serving as a SIB electrode,it exhibited an exceptional rate capability of 243.5 mAh·g^(-1)at 20 A·g^(-1).With the goal of developing high-performance PIB/SIB electrode materials,the proposed strategy,based on heterointerface adaptation engineering,is promising.
基金the Department of Science and Technology of Anhui Province(2022h11020024)Anhui Construction Engineering Group Co.,Ltd.(SG2025Q11)+4 种基金Basic Research Project from Institute of Coal Chemistry,CAS(SCJC-HN-2022-17)Shanxi Province Science Foundation(20210302124446202102070301018)The University Synergy Innovation Program of Anhui Province(GXXT-2022-27)Scientific Research Foundation for High-level Talents of Anhui University of Science and Technology(2023yjrc51)for funding。
文摘Sustainable H_(2) production based on hydrogen evolution reaction (HER) and hydrazine oxidation reaction (HzOR) has attracted wide attention due to minimal energy consumption compared to overall water electrolysis.The present study focuses on the design and construction of heterostructured CoPB@NiFe-OH applied as efficient bifunctional catalysts to sustainably produce hydrogen and remove hydrazine in alkaline media.Impressively,CoPB@NiFe-OH heterointerface exhibits an HzOR potential of-135 mV at the current density of 10 mA cm^(2) when the P to B atom ratio was 0.2,simultaneously an HER potential of-32 mV toward HER when the atom ratio of P and B was 0.5.Thus,hydrogen production without an outer voltage accompanied by a small current density output of 25 mA cm^(2) is achieved,surpassing most reported catalysts.In addition,DFT calculations demonstrate the Co sites in CoPB upgrades H*adsorption,while the Ni sites in NiFe-OH optimizes the adsorption energy of N_(2)H_(4)*due to electron transfer from CoPB to NiFe-OH at the heterointerface,ultimately leading to exceptional performance in hydrazine-assistant water electrolysis via HER coupled with HzOR.
