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
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
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
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
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
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
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
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
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
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
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
The buried heterointerface of perovskite solar cells(PSCs)suffers from serious nonradiative recombination and ultraviolet(UV)light stress,relentlessly limiting further increase in their power conversion efficiency and...The buried heterointerface of perovskite solar cells(PSCs)suffers from serious nonradiative recombination and ultraviolet(UV)light stress,relentlessly limiting further increase in their power conversion efficiency and operational stability.Herein,we develop an emerging strategy of incorporating a thin UV-activated tautomeric transition layer onto underlying charge transport layer and then depositing perovskite layer to construct an efficient hole-selective buried heterojunction.It is revealed that the UV-activated tautomeric transition interlayer not only improves upper perovskite crystallinity,diminishes thermionic loss for collecting hole and passivates defect site at such buried contact that significantly promote charge transport and suppress nonradiative recombination,but also effectively protects adjacent perovskite from UV degradation through“UV sunscreen”effect.As a result,we report a remarkably enhanced efficiency of 24.76%compared to 22.02%of the control device.More importantly,the achieved high-efficiency PSC features excellent resistance against UV radiation at 365 nm of 100 and 850 mW cm^(−2),which are approximately 21 and 184 times of UV flux(4.6 mW cm^(−2))under AM 1.5G solar illumination.This work provides a promising approach of strengthening buried heterointerface for simultaneous realization of highly efficient and UV robust PSCs.展开更多
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 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(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.
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supported by the National Natural Science Foundation of China(62322407,22279034,52261145698)the National Key Research and Development Program of China(2022YFB3803300)+1 种基金the Shanghai Science and Technology Innovation Action Plan(22ZR1418900)Xiong S thanks the project funded by China Postdoctoral Science Foundation(BX20220089,2022M720742).
文摘The buried heterointerface of perovskite solar cells(PSCs)suffers from serious nonradiative recombination and ultraviolet(UV)light stress,relentlessly limiting further increase in their power conversion efficiency and operational stability.Herein,we develop an emerging strategy of incorporating a thin UV-activated tautomeric transition layer onto underlying charge transport layer and then depositing perovskite layer to construct an efficient hole-selective buried heterojunction.It is revealed that the UV-activated tautomeric transition interlayer not only improves upper perovskite crystallinity,diminishes thermionic loss for collecting hole and passivates defect site at such buried contact that significantly promote charge transport and suppress nonradiative recombination,but also effectively protects adjacent perovskite from UV degradation through“UV sunscreen”effect.As a result,we report a remarkably enhanced efficiency of 24.76%compared to 22.02%of the control device.More importantly,the achieved high-efficiency PSC features excellent resistance against UV radiation at 365 nm of 100 and 850 mW cm^(−2),which are approximately 21 and 184 times of UV flux(4.6 mW cm^(−2))under AM 1.5G solar illumination.This work provides a promising approach of strengthening buried heterointerface for simultaneous realization of highly efficient and UV robust PSCs.
