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
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
Highly developed electronic information technology has undoubtedly resulted in numerous benefits to the military and public life.However,the resulting electromagnetic wave(EW)pollution cannot be ignored.Therefore,the ...Highly developed electronic information technology has undoubtedly resulted in numerous benefits to the military and public life.However,the resulting electromagnetic wave(EW)pollution cannot be ignored.Therefore,the application of highly efficient EW materials is becoming an important requirement.In this study,magnetic-dielectric heterointerface strategy was applied to construct absorbers with desirable electromagnetic wave properties.A novel CoO/Co nanoparticle anchored to N-doped mesoporous carbon(CoO/Co/N-CMK-3)composites was fabricated by facile precipitation reaction and the electromagnetic characteristics have been well optimized by adjusting pyrolysis temperature.The CoO/Co/N-CMK-3 yielded its highest performance at an annealing temperature of 800℃,with an extended effective absorption bandwidth of 5.83 GHz and unusually low minimum reflection loss of−63.82 dB,even at a thickness of just 1.8 mm and low filler loading(10%).For the excellent microwave absorption property,the advantages of the CoO/Co/N-CMK-3 can be summed up as follows.Firstly,the incorporation of heterointerfaces among N-CMK-3,CoO,and Co introduces abundant polarization centers,triggering various polarization effects and increasing dielectric losses.Secondly,the CoO/Co magnetic component introduced the strong magnetic loss and improved the impedance matching capability of CoO/Co/N-CMK-3.Thirdly,the extraordinary magnetic-dielectric behavior is supported by multiple magnetic coupling networks and enriched air-material heterointerfaces,boosted the magnetoelectric cooperative loss for further optimizing the electromagnetic dissipation and broadening the effective absorption frequency band.Moreover,the CST simulation results validate the impressive operational bandwidth and reflection loss characteristics of the obtained absorbers.This study demonstrates a novel heterointerface engineering strategy for designing lightweight,wide-band,and high-performance EW absorbers.展开更多
The adsorption-catalysis ability of metal-based catalysts toward lithium polysulfides(LiPSs)is dominated by the position of their d-/p-band center.An available strategy to strengthen the d-p band center proximity of m...The adsorption-catalysis ability of metal-based catalysts toward lithium polysulfides(LiPSs)is dominated by the position of their d-/p-band center.An available strategy to strengthen the d-p band center proximity of metal-based catalysts is to fabricate a crystalline-amorphous heterointerface,which markedly enhances LiPS conversion.The polyanionic pyrophosphate of TiP_(2)O_(7)serves as an efficient catalyst and ionic conductor for lithium-sulfur(Li-S)batteries.However,TiP_(2)O_(7)does not fully optimize sulfur redox reactivity due to limitations in factors such as the adsorption-catalysis of sulfur species,Li^(+)diffusion,and electron transfer.Herein,we engineer the crystalline-amorphous heterointerface of TiP_(2)O_(7)combined with carbon nanotubes(CNTs)to facilitate electronic donation from C to TiP_(2)O_(7).This interaction results in an upward shift of the Ti d,enhancing the proximity of the d-p band center in TiP_(2)O_(7)/CNTs.By utilizing TiP_(2)O_(7)/CNTs as both electrode and separator modifier,we optimize the LiPS conversion process,showing a comprehensive strategy to mitigate the diffusion of LiPSs and achieve the bidirectional redox reactions in Li-S batteries.Accordingly,the cell assembled by TiP_(2)O_(7)/CNTs delivers a satisfactory capacity of835 mAh g^(-1)after 300 cycles at 4 C and an impressive initial areal capacity of 3.52 mAh cm^(-2)under the sulfur areal loading of 5 mg cm^(-2)at 0.1 C.Additionally,the Li//Li cells utilizing TiP_(2)O_(7)/CNTs present a prolonged cycling life of up to 1800 h without voltage fluctuation and Li dendrite growth.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
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
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 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
Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxy...Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this work,we synthesized a self-supporting heterogeneous NiSe@Co_(0.85)Se/NF electrocatalyst using a facile in situ selenization of transition metal precursors that coated on the nickel foam(NF)in polyol solution.The NF was used as both conductive substrate and nickel source,ensuring superior electronic conductivity for catalyzing.The NiSe@-Co_(0.85)Se/NF exhibited remarkable bifunctional electrocatalytic activities with HER overpotential of 168 mV and OER overpotential of 258 mV to achieve 10 mA·cm-2.The water splitting system using NiSe@Co_(0.85)Se/NF as both anode and cathode electrodes achieved a current density of 10 mA·cm^(-2) at 1.61 V with nearly 100% faradaic efficiency and impressively long-term stability.The efficient bifunctional catalytic performance of NiSe@-Co_(0.85)Se/NF should be attributed to the electronic modulation and synergistic effect between NiSe and Co_(0.85)Se,the intrinsic metallic conductivity and the enlarged active sites exposure.This work provides a facile method for developing heterogeneous bifunctional catalysts for advanced electrochemical energy conversion technologies.展开更多
Manganese-based material is a prospective cathode material for aqueous zinc ion batteries(ZIBs)by virtue of its high theoretical capacity,high operating voltage,and low price.However,the manganese dissolution during t...Manganese-based material is a prospective cathode material for aqueous zinc ion batteries(ZIBs)by virtue of its high theoretical capacity,high operating voltage,and low price.However,the manganese dissolution during the electrochemical reaction causes its electrochemical cycling stability to be undesirable.In this work,heterointerface engineering-induced oxygen defects are introduced into heterostructure MnO_(2)(δa-MnO_(2))by in situ electrochemical activation to inhibit manganese dissolution for aqueous zinc ion batteries.Meanwhile,the heterointerface between the disordered amorphous and the crystalline MnO_(2)ofδa-MnO_(2)is decisive for the formation of oxygen defects.And the experimental results indicate that the manganese dissolution ofδa-MnO_(2)is considerably inhibited during the charge/discharge cycle.Theoretical analysis indicates that the oxygen defect regulates the electronic and band structure and the Mn-O bonding state of the electrode material,thereby promoting electron transport kinetics as well as inhibiting Mn dissolution.Consequently,the capacity ofδa-MnO_(2)does not degrade after 100 cycles at a current density of 0.5 Ag^(-1)and also 91%capacity retention after 500cycles at 1 Ag^(-1).This study provides a promising insight into the development of high-performance manganese-based cathode materials through a facile and low-cost strategy.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
Improving the cycling stability of metal sulfide-based anode materials at high rate is of great significance for advanced sodium ion batteries.However,the sluggish reaction kinetics is a big obstacle for the developme...Improving the cycling stability of metal sulfide-based anode materials at high rate is of great significance for advanced sodium ion batteries.However,the sluggish reaction kinetics is a big obstacle for the development of high-performance sodium storage electrodes.Herein,we have rationally engineered the heterointerface by designing the Fe1?xS/MoS2 heterostructure with abundant“ion reservoir”to endow the electrode with excellent cycling stability and rate capability,which is proved by a series of in and ex situ electrochemical investigations.Density functional theory calculations further reveal that the heterointerface greatly decreases sodium ion diffusion barrier and facilitates charge-transfer kinetics.Our present findings not only provide a deep analysis on the correlation between the structure and performance,but also draw inspiration for rational heterointerface engineering toward the next-generation high-performance energy storage devices.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
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
Cd1-xZnxS/Cu2ZnSnS4 （CZTS）-based thin film solar cells usually use CdS as a buffer layer, but due to its smaller band gap （2.4 eV）, CdS film has been replaced with higher band gap materials. The cadmium zinc sulfi...Cd1-xZnxS/Cu2ZnSnS4 （CZTS）-based thin film solar cells usually use CdS as a buffer layer, but due to its smaller band gap （2.4 eV）, CdS film has been replaced with higher band gap materials. The cadmium zinc sulfide （CdZnS） ternary compound has a higher band gap than other compounds, which leads to a decrease in window absorption loss. In this paper, the band offsets at Cd1-xZnxS/CuzZnSnS4 （CZTS） heterointerface are calculated by the first-principles, density- functional and pseudopotential method. The band offsets at Cdl xZnxS/CZTS heterointerface are tuned by controlling the composition of Zn in Cd1-xZnxS alloy, the calculated valence band offsets are small, which is consistent with the commonanion rule. The favorable heterointerface of type-I with a moderate barrier height （〈 0.3 eV） can be obtained by controlling the composition of Zn in Cdl-xZnxS alloy between 0.25 and 0.375.展开更多
Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix largely li...Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix largely limits the overall electrocatalytic performance due to their insufficient cooperative effects.Herein,we report a controllable and robust heterointerface engineering strategy for the bottom-up fabrication of rhombic Rh nanosheets in situ confined on Ti_3C_(2)T_x MXene nanolamellas(Rh NS/MXene)via a convenient stereoassembly process.This unique design concept gives the resulting 2D/2D Rh NS/MXene heterostructure intriguing textural features,including large accessible surface areas,strong"face-toface"interfacial interactions,homogeneous Rh nanosheet distribution,ameliorative electronic structure,and high electronic conductivity.As a consequence,the as-prepared Rh NS/MXene nanoarchitectures exhibit exceptional electrocatalytic methanol oxidation properties in terms of a large electrochemically active surface area of 126.2 m~2 g_(Rh)~(-1),a high mass activity of 1056.9 mA mg_(Rh)-~1,and a long service life,which significantly outperform those of conventional particle-shaped Rh catalysts supported by carbon black,carbon nanotubes,reduced graphene oxide,and MXene matrixes as well as the commercial Pt nanoparticle/carbon black and Pd nanoparticle/carbon black catalysts with the same noble metal loading amount.Density functional theory calculations further demonstrate that the direct electronic interaction at the well-contacted 2D/2D heterointerfaces effectively enhances the adsorption energy of Rh nanosheets and induces a left shift of the d-band center,thereby making the Rh NS/MXene configuration suffer less from CO poisoning.This work highlights the importance of rational heterointerface design in the construction of advanced noble metal/MXene electrocatalysts,which may provide new avenues for developing the next-generation DMFC devices.展开更多
Tailoring the electronic states of the Al N/diamond interface is critical to the development of the next-generation semiconductor devices such as the deep-ultraviolet light-emitting diode, photodetector, and high-powe...Tailoring the electronic states of the Al N/diamond interface is critical to the development of the next-generation semiconductor devices such as the deep-ultraviolet light-emitting diode, photodetector, and high-power high-frequency field-effect transistor. In this work, we investigate the electronic properties of the semipolar plane Al N（11^-01）/diamond heterointerfaces by using the first-principles method with regard to different terminated planes of Al N and surface structures of diamond（100） plane. A large number of gap states exist at semi-polar plane Al N（11^-01）/diamond heterointerface, which results from the N 2 p and C 2 s2 p orbital states. Besides, the charge transfer at the interface strongly depends on the surface termination of diamond, on which hydrogen suppresses the charge exchange at the interface. The band alignments of semi-polar plane Al N（11^-01）/diamond show a typical electronic character of the type-Ⅱ staggered band configuration. The hydrogen-termination of diamond markedly increases the band offset with a maximum valence band offset of 2.0 e V and a conduction band offset of 1.3 e V for the semi-polar plane N–Al N（11^-01）/hydrogenated diamond surface. The unique band alignment of this Type-Ⅱ staggered system with the higher CBO and VBO of the semi-polar Al N/HC（100） heterostructure provides an avenue to the development of robust high-power high-frequency power devices.展开更多
To promote the practices of perovskite photovoltaics,it requires to develop efficient perovskite solar cells(PVSCs)standing long-time operation under the adverse environments.Herein,we demonstrate that the tailor-made...To promote the practices of perovskite photovoltaics,it requires to develop efficient perovskite solar cells(PVSCs)standing long-time operation under the adverse environments.Herein,we demonstrate that the tailor-made conjugated polymers as conductive adhesives stabilized the originally redox-reactive heterointerface between perovskite and metal oxide,facilitating the access of efficient and stable inverted PVSCs.It was revealed that bithiophene and phenyl alternating conjugated polymers with partial glycol chains atop of the metal oxide layer has resulted in effective organic-inorganic hybrid hole transporting bilayers,which allow maintaining efficient hole extraction and transport,meanwhile preventing halide migration to directly contact with the nickel oxide(NiO_(x))layer.As a result,the corresponding inverted PVSCs with the organic-inorganic hole transporting bilayers have achieved an excellent power conversion efficiency of 23.22%,outperforming 20.65% of bare NiO_(x)-based devices.Moreover,the encapsulated PVSCs with organic-inorganic bilayers exhibited the excellent photostability with 91% of the initial efficiency after 1000-h one-sun equivalent illumination in ambient conditions.Overall,this work provides new insights into stabilizing the vulnerable heterointerface for perovskite solar cells.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.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.
基金financially supported by National Key Research and Development Program of China(Nos.2022YFB3807100 and 2022YFB3807101)National Science Fund for Distinguished Young Scholars(No.52025034)+3 种基金National Natural Science Foundation of China(No.22205182)Guangdong Basic and Applied Basic Re-search Foundation(No.2024A1515011516)China Postdoctoral Science Foundation(Nos.2022M722594 and 2024T171710)financially supported by Innovation Team of Shaanxi Sanqin Scholars.
文摘Highly developed electronic information technology has undoubtedly resulted in numerous benefits to the military and public life.However,the resulting electromagnetic wave(EW)pollution cannot be ignored.Therefore,the application of highly efficient EW materials is becoming an important requirement.In this study,magnetic-dielectric heterointerface strategy was applied to construct absorbers with desirable electromagnetic wave properties.A novel CoO/Co nanoparticle anchored to N-doped mesoporous carbon(CoO/Co/N-CMK-3)composites was fabricated by facile precipitation reaction and the electromagnetic characteristics have been well optimized by adjusting pyrolysis temperature.The CoO/Co/N-CMK-3 yielded its highest performance at an annealing temperature of 800℃,with an extended effective absorption bandwidth of 5.83 GHz and unusually low minimum reflection loss of−63.82 dB,even at a thickness of just 1.8 mm and low filler loading(10%).For the excellent microwave absorption property,the advantages of the CoO/Co/N-CMK-3 can be summed up as follows.Firstly,the incorporation of heterointerfaces among N-CMK-3,CoO,and Co introduces abundant polarization centers,triggering various polarization effects and increasing dielectric losses.Secondly,the CoO/Co magnetic component introduced the strong magnetic loss and improved the impedance matching capability of CoO/Co/N-CMK-3.Thirdly,the extraordinary magnetic-dielectric behavior is supported by multiple magnetic coupling networks and enriched air-material heterointerfaces,boosted the magnetoelectric cooperative loss for further optimizing the electromagnetic dissipation and broadening the effective absorption frequency band.Moreover,the CST simulation results validate the impressive operational bandwidth and reflection loss characteristics of the obtained absorbers.This study demonstrates a novel heterointerface engineering strategy for designing lightweight,wide-band,and high-performance EW absorbers.
基金supported by the National Natural Science Foundation of China(22278347)。
文摘The adsorption-catalysis ability of metal-based catalysts toward lithium polysulfides(LiPSs)is dominated by the position of their d-/p-band center.An available strategy to strengthen the d-p band center proximity of metal-based catalysts is to fabricate a crystalline-amorphous heterointerface,which markedly enhances LiPS conversion.The polyanionic pyrophosphate of TiP_(2)O_(7)serves as an efficient catalyst and ionic conductor for lithium-sulfur(Li-S)batteries.However,TiP_(2)O_(7)does not fully optimize sulfur redox reactivity due to limitations in factors such as the adsorption-catalysis of sulfur species,Li^(+)diffusion,and electron transfer.Herein,we engineer the crystalline-amorphous heterointerface of TiP_(2)O_(7)combined with carbon nanotubes(CNTs)to facilitate electronic donation from C to TiP_(2)O_(7).This interaction results in an upward shift of the Ti d,enhancing the proximity of the d-p band center in TiP_(2)O_(7)/CNTs.By utilizing TiP_(2)O_(7)/CNTs as both electrode and separator modifier,we optimize the LiPS conversion process,showing a comprehensive strategy to mitigate the diffusion of LiPSs and achieve the bidirectional redox reactions in Li-S batteries.Accordingly,the cell assembled by TiP_(2)O_(7)/CNTs delivers a satisfactory capacity of835 mAh g^(-1)after 300 cycles at 4 C and an impressive initial areal capacity of 3.52 mAh cm^(-2)under the sulfur areal loading of 5 mg cm^(-2)at 0.1 C.Additionally,the Li//Li cells utilizing TiP_(2)O_(7)/CNTs present a prolonged cycling life of up to 1800 h without voltage fluctuation and Li dendrite growth.
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 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(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(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(No.51804216)。
文摘Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this work,we synthesized a self-supporting heterogeneous NiSe@Co_(0.85)Se/NF electrocatalyst using a facile in situ selenization of transition metal precursors that coated on the nickel foam(NF)in polyol solution.The NF was used as both conductive substrate and nickel source,ensuring superior electronic conductivity for catalyzing.The NiSe@-Co_(0.85)Se/NF exhibited remarkable bifunctional electrocatalytic activities with HER overpotential of 168 mV and OER overpotential of 258 mV to achieve 10 mA·cm-2.The water splitting system using NiSe@Co_(0.85)Se/NF as both anode and cathode electrodes achieved a current density of 10 mA·cm^(-2) at 1.61 V with nearly 100% faradaic efficiency and impressively long-term stability.The efficient bifunctional catalytic performance of NiSe@-Co_(0.85)Se/NF should be attributed to the electronic modulation and synergistic effect between NiSe and Co_(0.85)Se,the intrinsic metallic conductivity and the enlarged active sites exposure.This work provides a facile method for developing heterogeneous bifunctional catalysts for advanced electrochemical energy conversion technologies.
基金funds from the National Natural Science Foundation of China(51772082 and 51804106)the Natural Science Foundation of Hunan Province(2023JJ10005)
文摘Manganese-based material is a prospective cathode material for aqueous zinc ion batteries(ZIBs)by virtue of its high theoretical capacity,high operating voltage,and low price.However,the manganese dissolution during the electrochemical reaction causes its electrochemical cycling stability to be undesirable.In this work,heterointerface engineering-induced oxygen defects are introduced into heterostructure MnO_(2)(δa-MnO_(2))by in situ electrochemical activation to inhibit manganese dissolution for aqueous zinc ion batteries.Meanwhile,the heterointerface between the disordered amorphous and the crystalline MnO_(2)ofδa-MnO_(2)is decisive for the formation of oxygen defects.And the experimental results indicate that the manganese dissolution ofδa-MnO_(2)is considerably inhibited during the charge/discharge cycle.Theoretical analysis indicates that the oxygen defect regulates the electronic and band structure and the Mn-O bonding state of the electrode material,thereby promoting electron transport kinetics as well as inhibiting Mn dissolution.Consequently,the capacity ofδa-MnO_(2)does not degrade after 100 cycles at a current density of 0.5 Ag^(-1)and also 91%capacity retention after 500cycles at 1 Ag^(-1).This study provides a promising insight into the development of high-performance manganese-based cathode materials through a facile and low-cost strategy.
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the support from the Thousand Young Talents Program of Chinathe National Natural Science Foundation of China(Nos.51602200,61874074,21603192)+3 种基金Science and Technology Project of Shenzhen(JCYJ20170817101100705,JCYJ20170817100111548,ZDSYS201707271014468)the(Key)Project of Department of Education of Guangdong Province(No.2016KZDXM008)supported by Shenzhen Peacock Plan(No.KQTD2016053112042971)Singapore Ministry of Education Academic Research Fund Tier 2(MOE2018-T2-2-178).
文摘Improving the cycling stability of metal sulfide-based anode materials at high rate is of great significance for advanced sodium ion batteries.However,the sluggish reaction kinetics is a big obstacle for the development of high-performance sodium storage electrodes.Herein,we have rationally engineered the heterointerface by designing the Fe1?xS/MoS2 heterostructure with abundant“ion reservoir”to endow the electrode with excellent cycling stability and rate capability,which is proved by a series of in and ex situ electrochemical investigations.Density functional theory calculations further reveal that the heterointerface greatly decreases sodium ion diffusion barrier and facilitates charge-transfer kinetics.Our present findings not only provide a deep analysis on the correlation between the structure and performance,but also draw inspiration for rational heterointerface engineering toward the next-generation high-performance energy storage devices.
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Project supported by the Special Funds of the National Natural Science Foundation of China(Grant Nos.11547226 and 11547180)
文摘Cd1-xZnxS/Cu2ZnSnS4 （CZTS）-based thin film solar cells usually use CdS as a buffer layer, but due to its smaller band gap （2.4 eV）, CdS film has been replaced with higher band gap materials. The cadmium zinc sulfide （CdZnS） ternary compound has a higher band gap than other compounds, which leads to a decrease in window absorption loss. In this paper, the band offsets at Cd1-xZnxS/CuzZnSnS4 （CZTS） heterointerface are calculated by the first-principles, density- functional and pseudopotential method. The band offsets at Cdl xZnxS/CZTS heterointerface are tuned by controlling the composition of Zn in Cd1-xZnxS alloy, the calculated valence band offsets are small, which is consistent with the commonanion rule. The favorable heterointerface of type-I with a moderate barrier height （〈 0.3 eV） can be obtained by controlling the composition of Zn in Cdl-xZnxS alloy between 0.25 and 0.375.
基金supported by the National Natural Science Foundation of China(11872171 and 22209037)the Project on Excellent Post-graduate Dissertation of Hohai University。
文摘Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix largely limits the overall electrocatalytic performance due to their insufficient cooperative effects.Herein,we report a controllable and robust heterointerface engineering strategy for the bottom-up fabrication of rhombic Rh nanosheets in situ confined on Ti_3C_(2)T_x MXene nanolamellas(Rh NS/MXene)via a convenient stereoassembly process.This unique design concept gives the resulting 2D/2D Rh NS/MXene heterostructure intriguing textural features,including large accessible surface areas,strong"face-toface"interfacial interactions,homogeneous Rh nanosheet distribution,ameliorative electronic structure,and high electronic conductivity.As a consequence,the as-prepared Rh NS/MXene nanoarchitectures exhibit exceptional electrocatalytic methanol oxidation properties in terms of a large electrochemically active surface area of 126.2 m~2 g_(Rh)~(-1),a high mass activity of 1056.9 mA mg_(Rh)-~1,and a long service life,which significantly outperform those of conventional particle-shaped Rh catalysts supported by carbon black,carbon nanotubes,reduced graphene oxide,and MXene matrixes as well as the commercial Pt nanoparticle/carbon black and Pd nanoparticle/carbon black catalysts with the same noble metal loading amount.Density functional theory calculations further demonstrate that the direct electronic interaction at the well-contacted 2D/2D heterointerfaces effectively enhances the adsorption energy of Rh nanosheets and induces a left shift of the d-band center,thereby making the Rh NS/MXene configuration suffer less from CO poisoning.This work highlights the importance of rational heterointerface design in the construction of advanced noble metal/MXene electrocatalysts,which may provide new avenues for developing the next-generation DMFC devices.
基金Project supported by the Scholarship Council of China(Grant No.201508340047)the Postdoctoral Science Foundation of China(Grant No.2016M601993)+1 种基金the Postdoctoral Science Foundation of Anhui Province,China(Grant No.2017B215)the Anhui Province University Outstanding Talent Cultivation Program,China(Grant No.gxfx ZD2016077)
文摘Tailoring the electronic states of the Al N/diamond interface is critical to the development of the next-generation semiconductor devices such as the deep-ultraviolet light-emitting diode, photodetector, and high-power high-frequency field-effect transistor. In this work, we investigate the electronic properties of the semipolar plane Al N（11^-01）/diamond heterointerfaces by using the first-principles method with regard to different terminated planes of Al N and surface structures of diamond（100） plane. A large number of gap states exist at semi-polar plane Al N（11^-01）/diamond heterointerface, which results from the N 2 p and C 2 s2 p orbital states. Besides, the charge transfer at the interface strongly depends on the surface termination of diamond, on which hydrogen suppresses the charge exchange at the interface. The band alignments of semi-polar plane Al N（11^-01）/diamond show a typical electronic character of the type-Ⅱ staggered band configuration. The hydrogen-termination of diamond markedly increases the band offset with a maximum valence band offset of 2.0 e V and a conduction band offset of 1.3 e V for the semi-polar plane N–Al N（11^-01）/hydrogenated diamond surface. The unique band alignment of this Type-Ⅱ staggered system with the higher CBO and VBO of the semi-polar Al N/HC（100） heterostructure provides an avenue to the development of robust high-power high-frequency power devices.
基金funded by the National Natural Science Foundation of China(No.22125901)the National Key Research and Development Program of China(No.2019YFA0705900)the Fundamental Research Funds for the Central Universities(No.226-2023-00113)。
文摘To promote the practices of perovskite photovoltaics,it requires to develop efficient perovskite solar cells(PVSCs)standing long-time operation under the adverse environments.Herein,we demonstrate that the tailor-made conjugated polymers as conductive adhesives stabilized the originally redox-reactive heterointerface between perovskite and metal oxide,facilitating the access of efficient and stable inverted PVSCs.It was revealed that bithiophene and phenyl alternating conjugated polymers with partial glycol chains atop of the metal oxide layer has resulted in effective organic-inorganic hybrid hole transporting bilayers,which allow maintaining efficient hole extraction and transport,meanwhile preventing halide migration to directly contact with the nickel oxide(NiO_(x))layer.As a result,the corresponding inverted PVSCs with the organic-inorganic hole transporting bilayers have achieved an excellent power conversion efficiency of 23.22%,outperforming 20.65% of bare NiO_(x)-based devices.Moreover,the encapsulated PVSCs with organic-inorganic bilayers exhibited the excellent photostability with 91% of the initial efficiency after 1000-h one-sun equivalent illumination in ambient conditions.Overall,this work provides new insights into stabilizing the vulnerable heterointerface for perovskite solar cells.
