TiO2 nanoparticles were prepared using the hydrothermal method and modified with CgN to syn-thesize a Type-Ⅱheterojunction semiconductor photocatalyst,TiO2-C;Na.In addition,a carbon layerwas coated onto the TiO2 nano...TiO2 nanoparticles were prepared using the hydrothermal method and modified with CgN to syn-thesize a Type-Ⅱheterojunction semiconductor photocatalyst,TiO2-C;Na.In addition,a carbon layerwas coated onto the TiO2 nanoparticles and the obtained material was uniformly covered on thesurface of CaNa to form an all-solid-state Z-scheme semiconductor photocatalyst,TiO2-C-C3N4,Through characterization by XRD,XPS,SEM,TEM,BET,photoelectrochemical experiments,UV-visible diffuse reflection,and PL spectroscopy,the charge transfer mechanism and band gappositions for the composite photocatalysts were analyzed.The Type-Ⅱand all-solid-state Z-schemeheterojunction structures were compared.By combining microscopic internal mechanisms withmacroscopic experimental phenomena,the relationship between performance and structure wasverified.Experimental methods were used to explore the adaptation degree of different photocata-lytic mechanisms using the same degradation system.This study highlights effective photocatalystdesign to meet the requirements for specific degradation conditions.展开更多
The rapid development of 5G communication technology and smart electronic and electrical equipment will inevitably lead to electromagnetic radiation pollution.Enriching heterointerface polarization relaxation through ...The rapid development of 5G communication technology and smart electronic and electrical equipment will inevitably lead to electromagnetic radiation pollution.Enriching heterointerface polarization relaxation through nanostructure design and interface modifica-tion has proven to be an effective strategy to obtain efficient electromagnetic wave absorption.Here,this work implements an innovative method that combines biomimetic honeycomb superstructure to constrain hierarchical porous heterostructure composed of Co/CoO nano-particles to improve the interfacial polarization intensity.The method effectively controlled the absorption efficiency of Co^(2+)through de-lignification modification of bamboo,and combined with the bionic carbon-based natural hierarchical porous structure to achieve uniform dispersion of nanoparticles,which is conducive to the in-depth construction of heterogeneous interfaces.In addition,the multiphase struc-ture brought about by high-temperature pyrolysis provides the best dielectric loss and impedance matching for the material.Therefore,the obtained bamboo-based Co/CoO multiphase composite showed excellent electromagnetic wave absorption performance,achieving excel-lent reflection loss(RL)of-79 dB and effective absorption band width of 4.12 GHz(6.84-10.96 GHz)at low load of 15wt%.Among them,the material’s optimal radar cross-section(RCS)reduction value can reach 31.9 dB·m^(2).This work provides a new approach to the micro-control and comprehensive optimization of macro-design of microwave absorbers,and offers new ideas for the high-value utiliza-tion of biomass materials.展开更多
In this study,a novel Ce-based metal-organic framework(Ce-OFDC)was synthesized via the hydrothermal method.To enhance its photocatalytic antimicrobial properties,polymeric carbon nitride(PCN)was incorporated into the ...In this study,a novel Ce-based metal-organic framework(Ce-OFDC)was synthesized via the hydrothermal method.To enhance its photocatalytic antimicrobial properties,polymeric carbon nitride(PCN)was incorporated into the Ce-OFDC matrix,forming a CeOFDC/PCN composite material.Antibacterial assays demonstrated that Ce-OFDC/PCN had significant inhibitory effects on both Escherichia coli(E.coli)and Staphylococcus aureus(S.aureus),achieving inhibition rates of 99.5%and 94.3%,respectively.Notably,the antibacterial performance of Ce-OFDC/PCN was superior to that of Ce-OFDC or PCN alone.Furthermore,photocurrent and electrical impedance scanning measurements demonstrated that the Ce-OFDC/PCN composites showed improved photocurrent response and superior efficiency in separating photogenerated electrons and holes.The photocurrent density of Ce-OFDC/PCN reached 120μA cm^(-2),which was 1.5 times higher than that of PCN(80μA cm^(-2))and 12 times higher than that of Ce-OFDC(10μA cm^(-2)).Electron paramagnetic resonance analysis indicated that reactive oxygen species played a crucial role in the antimicrobial process,with super oxide radicals(·O_(2)^(-))and hydroxyl radical(·OH)showing the most prominent influence.We conducted reactive oxygen species(ROS)scavenging experiments to further confirm this view.After adding glutathione(GSH)to remove all ROS,the antibacterial efficiency of Ce-OFDC/PCN decreased by about 40%.Adding D-mannitol to remove·OH reduced the inhibition rate to 54.7%,and adding superoxide dismutase(SOD)to remove·O_(2)^(-)reduced the inhibition rate to 65.4%.The Ce-OFDC/PCN heterostructure increased the separation efficiency of photogenerated electrons and holes,producing increased reactive oxygen species.That,in turn,contributed to the observed superior photocatalytic antibacterial performance.This research significantly advanced the development of metal-organic framework(MOF)-based materials and provided valuable insights into the design of antimicrobial photocatalysts.展开更多
Imines play a pivotal role as multifunctional intermediates in pharmaceutical and biological applications,and their selective synthesis under mild conditions has attracted increasing interest.In this study,a covalent-...Imines play a pivotal role as multifunctional intermediates in pharmaceutical and biological applications,and their selective synthesis under mild conditions has attracted increasing interest.In this study,a covalent-organic frameworks(COFs)modified with CeO_(2)quantum dots(QDs)were prepared through a simple chemical reaction using LZU1 COFs and Ce(NO_(3))_(3)·6H_(2)O serving as precursors.The optimized5CeO_(2)QDs@LZU1 decorated with about 3.9 wt%CeO_(2)QDs demonstrates excellent performance in the photocatalytic selective oxidative of amines in visible light conditions,achieving nearly 100%benzylamine conversion and over 99%imine selectivity within 6 h,which is significantly superior to that of pure LZU1 and CeO_(2).The remarkable enhancement in activity is mainly attributed to the fact that the interaction between CeO_(2)QDs and LZU1 COF in 5CeO_(2)QDs@LZU1 improves the visible light response and concurrently promotes the separation efficiency of photogenerated e-and h+pairs.Broad substrate scope also provides a prospect for the industrial synthesis of various imines.Our findings not only expand the application range of COFs by incorporating QDs but also lay the groundwork for their further rational design and optimization.展开更多
In order to obtain high-performance electromagnetic wave absorbers,the adjustment of structure and components is essential.Based on the above requirements,this system forms a three-dimensional frame structure consisti...In order to obtain high-performance electromagnetic wave absorbers,the adjustment of structure and components is essential.Based on the above requirements,this system forms a three-dimensional frame structure consisting of MXene and transition metal oxides(TMOs)through efficient electrostatic self-assembly.This three-dimensional network structure has rich heterojunction structures,which can cause a large amount of interface polarization and conduction losses in incident electromagnetic waves.Hollow structures cause multiple reflections and scattering of electromagnetic waves,which is also an important reason for further increasing electromagnetic wave losses.When the doping ratio is 1:1,the system has the best impedance matching,the maximum effective absorption bandwidth(EAB max)can reach 5.12 GHz at 1.7 mm,and the minimum reflection loss(RL_(min))is-50.30 dB at 1.8 mm.This provides a reference for the subsequent formation of 2D-MXene materials into 3D materials.展开更多
The aqueous rechargeable Zn-ion batteries based on the safe,low cost and environmental benignity aqueous electrolytes are one of the most compelling candidates for large scale energy storage applications.However,pursu...The aqueous rechargeable Zn-ion batteries based on the safe,low cost and environmental benignity aqueous electrolytes are one of the most compelling candidates for large scale energy storage applications.However,pursuing suitable insertion materials may be a great challenge due to the strong electrostatic interaction between Zn^(^(2+))and cathode materials.Hence,a novel NaV_(6)O_(15)/V_(2)O_(5) skin-core heterostructure nanowire is reported via a one-step hydrothermal method and subsequent calcination for high-stable aqueous Zn-ion batteries(ZIBs).The NaV_(6)O_(15)/V_(2)O_(5) cathode delivers high specific capacity of 390 m Ah/g at 0.3 A/g and outstanding cycling stability of 267 m Ah/g at 5 A/g with high capacity retention over 92.3%after 3000 cycles.The superior electrochemical performances are attributed to the synergistic effect of skin-core heterostructured NaV_(6)O_(15)/V_(2)O_(5),in which the sheath of NaV_(6)O_(15) possesses high stability and conductivity,and the V_(2)O_(5) endows high specific capacity.Besides,the heterojunction structure not only accelerates intercalation kinetics of Zn^(2+)transport but also further consolidates the stability of the layers of V_(2)O_(5) during the cyclic process.This work provides a new perspective in developing feasible insertion materials for rechargeable aqueous ZIBs.展开更多
Type‐II‐heterojunction TiO2nanorod arrays(NAs)are achieved by a combination of reduced and pristine TiO2NAs through a simple electrochemical reduction.The heterojunction‐structured TiO2NAs exhibit an enhanced photo...Type‐II‐heterojunction TiO2nanorod arrays(NAs)are achieved by a combination of reduced and pristine TiO2NAs through a simple electrochemical reduction.The heterojunction‐structured TiO2NAs exhibit an enhanced photo‐efficiency,with respect to those of pristine TiO2NAs and completely reduced black TiO2.The improved efficiency can be attributed to a synergistic effect of two contributions of the partially reduced TiO2NAs.The light absorption is significantly increased,from theUV to the visible spectrum.Moreover,the type II structure leads to enhanced separation and transport of the electrons and charges.The proposed electrochemical approach could be applied to various semiconductors for a control of the band structure and improved photoelectrochemical performance.展开更多
A top-contact organic field-effect transistor （OFET） is fabricated by adopting a pentacene/1,11-bis（di-4- tolylaminophenyl） cyclohexane （TAPC） heterojunction structure and inserting an MoO3 buffer layer between ...A top-contact organic field-effect transistor （OFET） is fabricated by adopting a pentacene/1,11-bis（di-4- tolylaminophenyl） cyclohexane （TAPC） heterojunction structure and inserting an MoO3 buffer layer between the TAPC organic semiconductor layer and the source/drain electrode. The performances of the heterojunction OFET, including output current, field-effect mobility, and threshed voltage~ are all significantly improved by introducing the MoO3 thin buffer layer. The performance improvement of the modified heterojunction OFET is attributed to a better contact formed at the Au/TAPC interface due to the MoO3 thin buffer layer, thereby leading to a remarkable reduction of the contact resistance at the metal/organic interface.展开更多
In order to advance the commercialization of rechargeable Li-air batteries,it is of importance to explore cathode catalyst with efficient catalytic activity.Transition metal oxides have poor electrical conductivity,wh...In order to advance the commercialization of rechargeable Li-air batteries,it is of importance to explore cathode catalyst with efficient catalytic activity.Transition metal oxides have poor electrical conductivity,while cobalt phosphide has excellent electrical conductivity and large specific surface area.Nevertheless,its application in organic Li-air batteries has been much less studied,and the electrocatalytic activity desires to be further elevated.Here,CoP/Co_(2)P heterojunction composite with higher polarity was fabricated.The discharge product of high-polarity CoP/Co_(2)P had a new porous box-like morphology,which was easy to be decomposed and exposed more active sites.The highly polar CoP/Co_(2)P heterostructure composite had homogeneous pores,the synergistic effect existed between CoP and Co_(2)P,and the discharge product was porous box mixed with Li_(2)O_(2)and LiOH,which made CoP/Co_(2)P achieve high specific capacity of14632 m Ah/g and cycle stably 161 times when used as air electrode cathode catalyst.This work furnished a thought for the construction of cathode catalysts with efficient catalytic activity for Li-air batteries.展开更多
The core-shell metastable intermolecular composites(MIC)have attracted much attention in the past few years due to their unique properties.Here,the preparation of Al-Core heterojunction fibers using PVP as a template ...The core-shell metastable intermolecular composites(MIC)have attracted much attention in the past few years due to their unique properties.Here,the preparation of Al-Core heterojunction fibers using PVP as a template is proposed.The nano-Al was directly added to the precursor solution of cupric acetate monohydrate(CAM)/Polyvinylpyrrolidone(PVP),and the initial Al@CAM/PVP fibers were obtained via electrospinning.The core-shell MIC fibers are then obtained by calcining the initial fibers.The morphology,structure,and composition of Al-core MIC fibers were characterized,that the energetic fibers calcined at 300℃,350℃,and 400℃have a core-shell structure with shell compositions CuxO and PVP,CuxO and Cu O,respectively.The energy release characteristics of Al-core MIC were investigated,and preliminary ignition tests were performed using an ignition temperature measuring instrument and a pulsed laser.The energetic fibers calcined at 300℃exhibited unique properties.The decomposition of PVP in the shell layer promoted exotherm,and a low-temperature exothermic peak was shown at 372-458℃.Lower ignition temperatures and higher flame heights were observed in the combustion tests than calcination at 350℃and 400℃.An unexpected result was that PVP can play a positive role in Al/CuO nanothermites.Simultaneously,this preparation method provided an idea for the integrated preparation of core-shell Al-Core MIC fibers and tuning the properties of MIC.展开更多
AgCl/Ti_(3)C_(2)@TiO_(2)ternary composites were prepared to form a heterojunction structure between AgCl and TiO_(2)and introduce Ti3C2 as a cocatalyst.The as-prepared AgCl/Ti_(3)C_(2)@TiO_(2)composites showed higher ...AgCl/Ti_(3)C_(2)@TiO_(2)ternary composites were prepared to form a heterojunction structure between AgCl and TiO_(2)and introduce Ti3C2 as a cocatalyst.The as-prepared AgCl/Ti_(3)C_(2)@TiO_(2)composites showed higher photocatalytic activity than pure AgCl and Ti_(3)C_(2)@TiO_(2)for photooxidation of a 1,4-dihydropyridine derivative(1,4-DHP)and tetracycline hydrochloride(TCH)under visible light irradiation(λ>400 nm).The photocatalytic activity of AgCl/Ti_(3)C_(2)@TiO_(2)composites depended on Ti_(3)C_(2)@TiO_(2)content,and the catalytic activity of the optimized samples were 6.9 times higher than that of pure AgCl for 1,4-DHP photodehydrogenation and 7.3 times higher than that of Ti_(3)C_(2)@TiO_(2)for TCH photooxidation.The increased photocatalytic activity was due to the formation of a heterojunction structure between AgCl and TiO_(2)and the introduction of Ti3C2 as a cocatalyst,which lowered the internal resistance,sped up the charge transfer,and increased the separation efficiency of photogenerated carries.Photogenerated holes and superoxide radical anions were the major active species in the photocatalytic process.展开更多
Organic electronic devices offer unique advantages in flexible,solution-processable,and cost-effective applications,where molecular stacking directly determines the optoelectronic properties of materials and devices.H...Organic electronic devices offer unique advantages in flexible,solution-processable,and cost-effective applications,where molecular stacking directly determines the optoelectronic properties of materials and devices.Heterojunction microstructures,which serve as the fundamental building blocks for controlling photoexciton dynamics and charge transport processes,have emerged as a critical feature to govern the coordination of exciton dynamics,charge transport,and multifunctional coupling in organic semiconductors.In this review,we provide a comprehensive overview of recent advances in heterojunction microstructures for modulating optoelectronic properties,offering valuable insights for high-performance and multifunctional organic electronics applications.We begin by introducing the fundamentals of heterojunction aggregation and its role in modulating physical processes through electronic structure and carrier transport engineering.Subsequently,we review recent progress in heterojunction aggregation within organic electronics,encompassing performance optimization and multifunctional extensions.In addition,we summarize four key strategies for constructing heterojunction microstructures in organic electronic devices.Finally,we outline future perspectives,emphasizing the critical need for deeper understanding of aggregation dynamics and the development of scalable fabrication approaches for heterojunction-structured films in next-generation intelligent devices.展开更多
Under the synergistic effect of molecular design and devices engineering, small molecular organic solar cells have presented an unstoppable tendency for rapid development with putting forward donor- acceptor （D-A） s...Under the synergistic effect of molecular design and devices engineering, small molecular organic solar cells have presented an unstoppable tendency for rapid development with putting forward donor- acceptor （D-A） structures. Up to now, the highest power conversion efficiency of small molecules has exceeded 11%, comparable to that of polymers. In this review, we summarize the high performance small molecule donors in various classes of typical donor-acceptor （D-A） structures and discuss their relationships briefly.展开更多
The development of hierarchical nanostructure is demonstrated as an effective strategy to improve catalytic activity and stability of electrocatalysts.Herein,a novel leaf-like hierarchically porous heterojunction flak...The development of hierarchical nanostructure is demonstrated as an effective strategy to improve catalytic activity and stability of electrocatalysts.Herein,a novel leaf-like hierarchically porous heterojunction flake arrays(FAs),integrated graphitic N-doped carbon(NC)with amorphous B,N-doped carbon(BNC),has been designed and grown on flexible carbon fiber(CF)using metal-organic framework(MOF)FAs and green ionic liquids as precursors.The hierarchical heterojunction structure possesses micro-and nano-scaled pores,large surface areas,and exposed high-density catalytic active sites,which enhances electronic conductivity and offers accessible transport channels for effectively decreasing mass transport resistance.The results of discrete Fourier transform(DFT)calculations and experiments also suggest that the catalytic activity has been promoted by the heterojunction structure through narrowing the banding gap.Consequently,the resultant nanohybrid microelectrode exhibits remarkable electrochemical sensing performance towards H2O2 with a low detection limit of 50 nM,and a high sensitivity of 213μA×mM-1×cm-2,as well as good anti-interference capability.The practical application of nanohybrid fiber microelectrode has been explored by real-time monitoring H2O2 released from live colon cells and surgically-resected fresh colon cancer tissue,which can provide important information for the identification of different types of cells as well as distinguish cancer cells from normal ones.We believe this research will pave the way towards the development of advanced carbon nanomaterials for application in the fields of electrochemistry,biosensing,and cancer diagnosis.展开更多
Exploring a new strategy for the removal of adsorbed CO (CO^(*)) on a Pt surface at a low potential is the key to achieving enhanced catalysis for the formic acid oxidation reaction (FAOR);however, the development of ...Exploring a new strategy for the removal of adsorbed CO (CO^(*)) on a Pt surface at a low potential is the key to achieving enhanced catalysis for the formic acid oxidation reaction (FAOR);however, the development of such a strategy remains a significant challenge. Herein, we report a class of Au/PtCo heterojunction nanowires (HNWs) as efficient electrocatalysts for accelerating the FAOR. This heterojunction structure and the induced Co alloying effects can facilitate formic acid adsorption/activation on Pt with high CO tolerance, generating the FAOR pathway from dehydration to dehydrogenation. The optimized Au_(23)/Pt_(63)Co_(14) HNWs showed the highest specific and mass activities of 11.7 mA cm^(−2)Pt and 6.42 A mg^(−1)Pt reported to date, respectively, which are considerably higher than those of commercial Pt/C. DFT calculations confirmed that the electron-rich Au segment enhances the electronic activity of the PtCo NWs, which not only allows the construction of a highly efficient electron transfer channel for the FAOR but also suppresses CO formation.展开更多
Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based...Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based on the results of density function theory calculations,a dual heterogeneous interfacial structured NiSe/Fe-Ni(OH)_(2)catalyst was subtly designed and successfully prepared by electrodepositing Fe-doped Ni(OH)_(2)on NiSe-loaded nickel foam(NF).Fe doping-driven heterogeneous structures in NiSe/Fe-Ni(OH)_(2)markedly boost catalytic activity and durability at industrially compatible current densities in single hydrogen and oxygen evolution reactions under alkaline conditions.In particular,NiSe/Fe-Ni(OH)_(2)shows a negligible performance loss at 600 mA cm^(-2)at least 1,000 h for overall water splitting,a distinguished long-term durability acting as AEMWE electrodes at 600 mA cm^(-2)and 1 A cm^(-2)at 85℃for at least 95 h.Owing to Fe doping-induced strong synergetic effect between Ni and Fe,dual heterostructure-promoted charge transfer and redistribution,abundant catalytic active sites,and improvement of stability and durability,a mechanism of Fe doping-driven heterogeneous interfacial structurepromoted catalytic performance was proposed.This study provides a successful example of theory-directed catalyst preparation and pioneers a creative strategy for industry-compatible water splitting at high current density.展开更多
文摘TiO2 nanoparticles were prepared using the hydrothermal method and modified with CgN to syn-thesize a Type-Ⅱheterojunction semiconductor photocatalyst,TiO2-C;Na.In addition,a carbon layerwas coated onto the TiO2 nanoparticles and the obtained material was uniformly covered on thesurface of CaNa to form an all-solid-state Z-scheme semiconductor photocatalyst,TiO2-C-C3N4,Through characterization by XRD,XPS,SEM,TEM,BET,photoelectrochemical experiments,UV-visible diffuse reflection,and PL spectroscopy,the charge transfer mechanism and band gappositions for the composite photocatalysts were analyzed.The Type-Ⅱand all-solid-state Z-schemeheterojunction structures were compared.By combining microscopic internal mechanisms withmacroscopic experimental phenomena,the relationship between performance and structure wasverified.Experimental methods were used to explore the adaptation degree of different photocata-lytic mechanisms using the same degradation system.This study highlights effective photocatalystdesign to meet the requirements for specific degradation conditions.
基金supported by the National Key R&D Program of China(Nos.2023YFE0108300 and 2023YFD2202103)the National Natural Science Foundation of China(No.32371972)+2 种基金the Natural Science Foundation of Jiangsu Province,China(No.BK20221336)Jiangsu Agricultural Science and Technology Independent Innovation Fund,China(No.CX(23)3060)Jiangxi Forestry Bureau Forestry Science and Technology Innovation Special Project,China(No.202240).
文摘The rapid development of 5G communication technology and smart electronic and electrical equipment will inevitably lead to electromagnetic radiation pollution.Enriching heterointerface polarization relaxation through nanostructure design and interface modifica-tion has proven to be an effective strategy to obtain efficient electromagnetic wave absorption.Here,this work implements an innovative method that combines biomimetic honeycomb superstructure to constrain hierarchical porous heterostructure composed of Co/CoO nano-particles to improve the interfacial polarization intensity.The method effectively controlled the absorption efficiency of Co^(2+)through de-lignification modification of bamboo,and combined with the bionic carbon-based natural hierarchical porous structure to achieve uniform dispersion of nanoparticles,which is conducive to the in-depth construction of heterogeneous interfaces.In addition,the multiphase struc-ture brought about by high-temperature pyrolysis provides the best dielectric loss and impedance matching for the material.Therefore,the obtained bamboo-based Co/CoO multiphase composite showed excellent electromagnetic wave absorption performance,achieving excel-lent reflection loss(RL)of-79 dB and effective absorption band width of 4.12 GHz(6.84-10.96 GHz)at low load of 15wt%.Among them,the material’s optimal radar cross-section(RCS)reduction value can reach 31.9 dB·m^(2).This work provides a new approach to the micro-control and comprehensive optimization of macro-design of microwave absorbers,and offers new ideas for the high-value utiliza-tion of biomass materials.
基金financially supported by the Youth Fund of the National Natural Science Foundation of China(No.22406161)“Lvyang Jinfeng Project”Funded by Yangzhou City(No.137013435)+2 种基金the Innovative Science and Technology Platform Project of Cooperation between Yangzhou City and Yangzhou Universitythe Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.SJCX23_1910)JST ACT-C program of Japan
文摘In this study,a novel Ce-based metal-organic framework(Ce-OFDC)was synthesized via the hydrothermal method.To enhance its photocatalytic antimicrobial properties,polymeric carbon nitride(PCN)was incorporated into the Ce-OFDC matrix,forming a CeOFDC/PCN composite material.Antibacterial assays demonstrated that Ce-OFDC/PCN had significant inhibitory effects on both Escherichia coli(E.coli)and Staphylococcus aureus(S.aureus),achieving inhibition rates of 99.5%and 94.3%,respectively.Notably,the antibacterial performance of Ce-OFDC/PCN was superior to that of Ce-OFDC or PCN alone.Furthermore,photocurrent and electrical impedance scanning measurements demonstrated that the Ce-OFDC/PCN composites showed improved photocurrent response and superior efficiency in separating photogenerated electrons and holes.The photocurrent density of Ce-OFDC/PCN reached 120μA cm^(-2),which was 1.5 times higher than that of PCN(80μA cm^(-2))and 12 times higher than that of Ce-OFDC(10μA cm^(-2)).Electron paramagnetic resonance analysis indicated that reactive oxygen species played a crucial role in the antimicrobial process,with super oxide radicals(·O_(2)^(-))and hydroxyl radical(·OH)showing the most prominent influence.We conducted reactive oxygen species(ROS)scavenging experiments to further confirm this view.After adding glutathione(GSH)to remove all ROS,the antibacterial efficiency of Ce-OFDC/PCN decreased by about 40%.Adding D-mannitol to remove·OH reduced the inhibition rate to 54.7%,and adding superoxide dismutase(SOD)to remove·O_(2)^(-)reduced the inhibition rate to 65.4%.The Ce-OFDC/PCN heterostructure increased the separation efficiency of photogenerated electrons and holes,producing increased reactive oxygen species.That,in turn,contributed to the observed superior photocatalytic antibacterial performance.This research significantly advanced the development of metal-organic framework(MOF)-based materials and provided valuable insights into the design of antimicrobial photocatalysts.
基金Project supported by the National Natural Science Foundation of China(22176054,22306060)China Postdoctoral Science Foundation(2022M721134)the Fundamental Research Funds for the Central Universities(2023MS060)。
文摘Imines play a pivotal role as multifunctional intermediates in pharmaceutical and biological applications,and their selective synthesis under mild conditions has attracted increasing interest.In this study,a covalent-organic frameworks(COFs)modified with CeO_(2)quantum dots(QDs)were prepared through a simple chemical reaction using LZU1 COFs and Ce(NO_(3))_(3)·6H_(2)O serving as precursors.The optimized5CeO_(2)QDs@LZU1 decorated with about 3.9 wt%CeO_(2)QDs demonstrates excellent performance in the photocatalytic selective oxidative of amines in visible light conditions,achieving nearly 100%benzylamine conversion and over 99%imine selectivity within 6 h,which is significantly superior to that of pure LZU1 and CeO_(2).The remarkable enhancement in activity is mainly attributed to the fact that the interaction between CeO_(2)QDs and LZU1 COF in 5CeO_(2)QDs@LZU1 improves the visible light response and concurrently promotes the separation efficiency of photogenerated e-and h+pairs.Broad substrate scope also provides a prospect for the industrial synthesis of various imines.Our findings not only expand the application range of COFs by incorporating QDs but also lay the groundwork for their further rational design and optimization.
基金supported by the National Natural Science Foundation of China(Nos.51407134,52002196)Natural Science Foundation of Shandong Province(Nos.ZR2019YQ24,ZR2020QF084)+1 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)and Special Financial of Shandong Province(Structural Design of High-efficiency Electromagnetic Wave-absorbing Composite Materials and Construction of Shandong Provincial Talent Teams(No.37000022P990304116449)).
文摘In order to obtain high-performance electromagnetic wave absorbers,the adjustment of structure and components is essential.Based on the above requirements,this system forms a three-dimensional frame structure consisting of MXene and transition metal oxides(TMOs)through efficient electrostatic self-assembly.This three-dimensional network structure has rich heterojunction structures,which can cause a large amount of interface polarization and conduction losses in incident electromagnetic waves.Hollow structures cause multiple reflections and scattering of electromagnetic waves,which is also an important reason for further increasing electromagnetic wave losses.When the doping ratio is 1:1,the system has the best impedance matching,the maximum effective absorption bandwidth(EAB max)can reach 5.12 GHz at 1.7 mm,and the minimum reflection loss(RL_(min))is-50.30 dB at 1.8 mm.This provides a reference for the subsequent formation of 2D-MXene materials into 3D materials.
基金the financial support from the National Natural Science Foundation of China(Nos.21878231 and 51603145)the Tianjin Natural Science Foundation of China(Nos.17JC ZDJ38100 and 19JCZDJC37300)+2 种基金the Science and Technology Plans of Tianjin(Nos.17PT SYJC00040 and 18PTSY JC00180)the China National Textile and Apparel Council(J201406)the China Petroleum Chemical Co Technology Development Project(216090 and 218008-6)。
文摘The aqueous rechargeable Zn-ion batteries based on the safe,low cost and environmental benignity aqueous electrolytes are one of the most compelling candidates for large scale energy storage applications.However,pursuing suitable insertion materials may be a great challenge due to the strong electrostatic interaction between Zn^(^(2+))and cathode materials.Hence,a novel NaV_(6)O_(15)/V_(2)O_(5) skin-core heterostructure nanowire is reported via a one-step hydrothermal method and subsequent calcination for high-stable aqueous Zn-ion batteries(ZIBs).The NaV_(6)O_(15)/V_(2)O_(5) cathode delivers high specific capacity of 390 m Ah/g at 0.3 A/g and outstanding cycling stability of 267 m Ah/g at 5 A/g with high capacity retention over 92.3%after 3000 cycles.The superior electrochemical performances are attributed to the synergistic effect of skin-core heterostructured NaV_(6)O_(15)/V_(2)O_(5),in which the sheath of NaV_(6)O_(15) possesses high stability and conductivity,and the V_(2)O_(5) endows high specific capacity.Besides,the heterojunction structure not only accelerates intercalation kinetics of Zn^(2+)transport but also further consolidates the stability of the layers of V_(2)O_(5) during the cyclic process.This work provides a new perspective in developing feasible insertion materials for rechargeable aqueous ZIBs.
基金supported from the National Natural Science Foundation of China (21425309, 21761132002, 21703040)China Postdoctoral Science Foundation (2017M622051) the 111 Project~~
文摘Type‐II‐heterojunction TiO2nanorod arrays(NAs)are achieved by a combination of reduced and pristine TiO2NAs through a simple electrochemical reduction.The heterojunction‐structured TiO2NAs exhibit an enhanced photo‐efficiency,with respect to those of pristine TiO2NAs and completely reduced black TiO2.The improved efficiency can be attributed to a synergistic effect of two contributions of the partially reduced TiO2NAs.The light absorption is significantly increased,from theUV to the visible spectrum.Moreover,the type II structure leads to enhanced separation and transport of the electrons and charges.The proposed electrochemical approach could be applied to various semiconductors for a control of the band structure and improved photoelectrochemical performance.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 61071026 and 61177032)the Science Fund for Creative Research Groups of the National Natural Science Foundation of China (Grant No.61021061)+1 种基金the Fundamental Research Fund for the Central Universities of Misistry of Education of China (Grant No.ZYGX2010Z004)the Specialized Research Fund for the Doctoral Program of Higher Education of China (Grant No. 20090185110020)
文摘A top-contact organic field-effect transistor （OFET） is fabricated by adopting a pentacene/1,11-bis（di-4- tolylaminophenyl） cyclohexane （TAPC） heterojunction structure and inserting an MoO3 buffer layer between the TAPC organic semiconductor layer and the source/drain electrode. The performances of the heterojunction OFET, including output current, field-effect mobility, and threshed voltage~ are all significantly improved by introducing the MoO3 thin buffer layer. The performance improvement of the modified heterojunction OFET is attributed to a better contact formed at the Au/TAPC interface due to the MoO3 thin buffer layer, thereby leading to a remarkable reduction of the contact resistance at the metal/organic interface.
基金supported by the National Science Foundations of China(Nos.21871028,22271018)。
文摘In order to advance the commercialization of rechargeable Li-air batteries,it is of importance to explore cathode catalyst with efficient catalytic activity.Transition metal oxides have poor electrical conductivity,while cobalt phosphide has excellent electrical conductivity and large specific surface area.Nevertheless,its application in organic Li-air batteries has been much less studied,and the electrocatalytic activity desires to be further elevated.Here,CoP/Co_(2)P heterojunction composite with higher polarity was fabricated.The discharge product of high-polarity CoP/Co_(2)P had a new porous box-like morphology,which was easy to be decomposed and exposed more active sites.The highly polar CoP/Co_(2)P heterostructure composite had homogeneous pores,the synergistic effect existed between CoP and Co_(2)P,and the discharge product was porous box mixed with Li_(2)O_(2)and LiOH,which made CoP/Co_(2)P achieve high specific capacity of14632 m Ah/g and cycle stably 161 times when used as air electrode cathode catalyst.This work furnished a thought for the construction of cathode catalysts with efficient catalytic activity for Li-air batteries.
文摘The core-shell metastable intermolecular composites(MIC)have attracted much attention in the past few years due to their unique properties.Here,the preparation of Al-Core heterojunction fibers using PVP as a template is proposed.The nano-Al was directly added to the precursor solution of cupric acetate monohydrate(CAM)/Polyvinylpyrrolidone(PVP),and the initial Al@CAM/PVP fibers were obtained via electrospinning.The core-shell MIC fibers are then obtained by calcining the initial fibers.The morphology,structure,and composition of Al-core MIC fibers were characterized,that the energetic fibers calcined at 300℃,350℃,and 400℃have a core-shell structure with shell compositions CuxO and PVP,CuxO and Cu O,respectively.The energy release characteristics of Al-core MIC were investigated,and preliminary ignition tests were performed using an ignition temperature measuring instrument and a pulsed laser.The energetic fibers calcined at 300℃exhibited unique properties.The decomposition of PVP in the shell layer promoted exotherm,and a low-temperature exothermic peak was shown at 372-458℃.Lower ignition temperatures and higher flame heights were observed in the combustion tests than calcination at 350℃and 400℃.An unexpected result was that PVP can play a positive role in Al/CuO nanothermites.Simultaneously,this preparation method provided an idea for the integrated preparation of core-shell Al-Core MIC fibers and tuning the properties of MIC.
基金This work was supported by the Opening Project of the Key Laboratory of Green Chemistry of Sichuan Institutes of Higher Education(LZJ2002)the Open Project of Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province(CSPC2016-3-2).
文摘AgCl/Ti_(3)C_(2)@TiO_(2)ternary composites were prepared to form a heterojunction structure between AgCl and TiO_(2)and introduce Ti3C2 as a cocatalyst.The as-prepared AgCl/Ti_(3)C_(2)@TiO_(2)composites showed higher photocatalytic activity than pure AgCl and Ti_(3)C_(2)@TiO_(2)for photooxidation of a 1,4-dihydropyridine derivative(1,4-DHP)and tetracycline hydrochloride(TCH)under visible light irradiation(λ>400 nm).The photocatalytic activity of AgCl/Ti_(3)C_(2)@TiO_(2)composites depended on Ti_(3)C_(2)@TiO_(2)content,and the catalytic activity of the optimized samples were 6.9 times higher than that of pure AgCl for 1,4-DHP photodehydrogenation and 7.3 times higher than that of Ti_(3)C_(2)@TiO_(2)for TCH photooxidation.The increased photocatalytic activity was due to the formation of a heterojunction structure between AgCl and TiO_(2)and the introduction of Ti3C2 as a cocatalyst,which lowered the internal resistance,sped up the charge transfer,and increased the separation efficiency of photogenerated carries.Photogenerated holes and superoxide radical anions were the major active species in the photocatalytic process.
基金supported by the National Natural Science Foundation(92477142)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0520203)+1 种基金the Beijing Municipal Natural Science Foundation(Z220025)the Fundamental Research Funds for the Central Universities.
文摘Organic electronic devices offer unique advantages in flexible,solution-processable,and cost-effective applications,where molecular stacking directly determines the optoelectronic properties of materials and devices.Heterojunction microstructures,which serve as the fundamental building blocks for controlling photoexciton dynamics and charge transport processes,have emerged as a critical feature to govern the coordination of exciton dynamics,charge transport,and multifunctional coupling in organic semiconductors.In this review,we provide a comprehensive overview of recent advances in heterojunction microstructures for modulating optoelectronic properties,offering valuable insights for high-performance and multifunctional organic electronics applications.We begin by introducing the fundamentals of heterojunction aggregation and its role in modulating physical processes through electronic structure and carrier transport engineering.Subsequently,we review recent progress in heterojunction aggregation within organic electronics,encompassing performance optimization and multifunctional extensions.In addition,we summarize four key strategies for constructing heterojunction microstructures in organic electronic devices.Finally,we outline future perspectives,emphasizing the critical need for deeper understanding of aggregation dynamics and the development of scalable fabrication approaches for heterojunction-structured films in next-generation intelligent devices.
基金supported by the National Natural Science Foundation of China (Nos. 21474022, 51603051)Youth Innovation Promotion Association CAS and Beijing Nova Program (No. Z171100001117062)the Chinese Academy of Sciences
文摘Under the synergistic effect of molecular design and devices engineering, small molecular organic solar cells have presented an unstoppable tendency for rapid development with putting forward donor- acceptor （D-A） structures. Up to now, the highest power conversion efficiency of small molecules has exceeded 11%, comparable to that of polymers. In this review, we summarize the high performance small molecule donors in various classes of typical donor-acceptor （D-A） structures and discuss their relationships briefly.
基金This work is supported by the National Natural Science Foundation of China(Nos.81572866,81773104,81773263,81873931,and 81974382)the China Postdoctoral Science Foundation(No.2019M652617)the National Key Basic Research Program of China(No.2015CB5540007).
文摘The development of hierarchical nanostructure is demonstrated as an effective strategy to improve catalytic activity and stability of electrocatalysts.Herein,a novel leaf-like hierarchically porous heterojunction flake arrays(FAs),integrated graphitic N-doped carbon(NC)with amorphous B,N-doped carbon(BNC),has been designed and grown on flexible carbon fiber(CF)using metal-organic framework(MOF)FAs and green ionic liquids as precursors.The hierarchical heterojunction structure possesses micro-and nano-scaled pores,large surface areas,and exposed high-density catalytic active sites,which enhances electronic conductivity and offers accessible transport channels for effectively decreasing mass transport resistance.The results of discrete Fourier transform(DFT)calculations and experiments also suggest that the catalytic activity has been promoted by the heterojunction structure through narrowing the banding gap.Consequently,the resultant nanohybrid microelectrode exhibits remarkable electrochemical sensing performance towards H2O2 with a low detection limit of 50 nM,and a high sensitivity of 213μA×mM-1×cm-2,as well as good anti-interference capability.The practical application of nanohybrid fiber microelectrode has been explored by real-time monitoring H2O2 released from live colon cells and surgically-resected fresh colon cancer tissue,which can provide important information for the identification of different types of cells as well as distinguish cancer cells from normal ones.We believe this research will pave the way towards the development of advanced carbon nanomaterials for application in the fields of electrochemistry,biosensing,and cancer diagnosis.
基金The authors are grateful for the financial support of this work from the National Science Fund for Distinguished Young Scholars(No.52025133)Tencent Foundation through the XPLORER PRIZE,the Beijing Natural Science Foundation(JQ18005)Young Thousand Talented Program,and Postdoctoral Science Foundation of China.(2020M680200).
文摘Exploring a new strategy for the removal of adsorbed CO (CO^(*)) on a Pt surface at a low potential is the key to achieving enhanced catalysis for the formic acid oxidation reaction (FAOR);however, the development of such a strategy remains a significant challenge. Herein, we report a class of Au/PtCo heterojunction nanowires (HNWs) as efficient electrocatalysts for accelerating the FAOR. This heterojunction structure and the induced Co alloying effects can facilitate formic acid adsorption/activation on Pt with high CO tolerance, generating the FAOR pathway from dehydration to dehydrogenation. The optimized Au_(23)/Pt_(63)Co_(14) HNWs showed the highest specific and mass activities of 11.7 mA cm^(−2)Pt and 6.42 A mg^(−1)Pt reported to date, respectively, which are considerably higher than those of commercial Pt/C. DFT calculations confirmed that the electron-rich Au segment enhances the electronic activity of the PtCo NWs, which not only allows the construction of a highly efficient electron transfer channel for the FAOR but also suppresses CO formation.
基金supported by the National Natural Science Foundation of China(22162025,22068037)the Youth Innovation Team of Shaanxi Universities+2 种基金the Open and Innovation Fund of Hubei Three Gorges Laboratory(SK232001)the Regional Innovation Capability Leading Program of Shaanxi(2022QFY07-03,2022QFY07-06)the Shaanxi Province Training Program of Innovation and Entrepreneurship for Undergraduates(S202210719108)。
文摘Developing highly stable electrocatalysts under industry-compatible current densities(>500 mA cm^(-2))in an anion-exchange membrane water electrolyzer(AEMWE)is an enormous challenge for water splitting.Herein,based on the results of density function theory calculations,a dual heterogeneous interfacial structured NiSe/Fe-Ni(OH)_(2)catalyst was subtly designed and successfully prepared by electrodepositing Fe-doped Ni(OH)_(2)on NiSe-loaded nickel foam(NF).Fe doping-driven heterogeneous structures in NiSe/Fe-Ni(OH)_(2)markedly boost catalytic activity and durability at industrially compatible current densities in single hydrogen and oxygen evolution reactions under alkaline conditions.In particular,NiSe/Fe-Ni(OH)_(2)shows a negligible performance loss at 600 mA cm^(-2)at least 1,000 h for overall water splitting,a distinguished long-term durability acting as AEMWE electrodes at 600 mA cm^(-2)and 1 A cm^(-2)at 85℃for at least 95 h.Owing to Fe doping-induced strong synergetic effect between Ni and Fe,dual heterostructure-promoted charge transfer and redistribution,abundant catalytic active sites,and improvement of stability and durability,a mechanism of Fe doping-driven heterogeneous interfacial structurepromoted catalytic performance was proposed.This study provides a successful example of theory-directed catalyst preparation and pioneers a creative strategy for industry-compatible water splitting at high current density.
基金supported by the National Key R&D Program of China(2022YFB3605402 and 2021YFB3601800)the Fundamental Research Funds for the Central Universities+3 种基金the National Natural Science Foundation of China(62274132,62004151,62274126,and 62174123)the Natural Science Basic Research Program of Shaanxi(2021JC24)the Innovation Capability Support Program of Shaanxi(2021TD-04)Wuhu and Xidian University Special Fund for Industry-university-research Cooperation(XWYCXY-012021001 and XWYCXY-012021006)。
