Organic molecule passivation of perovskite surfaces has emerged as a promising strategy for efficient and durable perovskite solar cells(PSCs).While many materials have been reported,the optimization of molecular stru...Organic molecule passivation of perovskite surfaces has emerged as a promising strategy for efficient and durable perovskite solar cells(PSCs).While many materials have been reported,the optimization of molecular structure for the best passivation effect remains of significant interest but lacks sufficient study.In this work,we designed and synthesized three novel donor–acceptor-donor(D-A-D)type conjugated organic small molecules with varying alkyl chain lengths to regulate the interface between perovskite and Spiro-OMeTAD.Among them,the OSIT molecule,which features an n-octyl side chain of optimal length,demonstrated a balanced interfacial contact and interaction with the perovskite surface.Beyond the passivation effect of the electron-rich C=O group on undercoordinated Pb2+defects,OSIT optimizes energy level alignment and improves charge extraction by acting as an efficient hole transport channel.As a result,PSCs with OSIT interfacial layer achieved an exceptional efficiency of 25.48%and a high open-circuit voltage of 1.18 V.Furthermore,the durability of unencapsulated devices was significantly enhanced under various environmental conditions,maintaining 93.7%of their initial efficiency after 1000 h of maximum power point tracking in a nitrogen atmosphere.This study provides valuable insights into the rational design of D-A-D type materials for effective interface modification in PSCs.展开更多
All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices,while their application is still in the initial stage.Here,a metal halide doping strategy was implem...All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices,while their application is still in the initial stage.Here,a metal halide doping strategy was implemented to enhance device performance and stability for inverted CsPbI_(3)perovskite solar cells(PSCs),which are ideal for integration into perovskite/silicon tandem solar cells.The lanthanide compound terbium chloride(TbCl_(3))was employed to improve buried interface between[4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)and perovskite layer,thereby enhancing the crystallinity of CsPbI_(3)films and passivating non-radiative recombination defects.Thus,the inverted CsPbI_(3)PSCs achieved an efficiency of 18.68%and demonstrated excellent stability against water and oxygen.Meanwhile,remarkable efficiencies of 29.40%and 25.44%were,respectively,achieved in four-terminal(4T)and two-terminal(2T)perovskite/silicon mechanically tandem devices,which are higher efficiencies among reported all-inorganic perovskite-based tandem solar cells.This study presents a novel approach for fabricating highly efficient and stable inverted all-inorganic PSCs and perovskite/silicon tandem solar cells.展开更多
Carbon nanotubes(CNTs)reinforced aluminum matrix composites(AMCs)show broad application prospects in the fields of aerospace and transportation because of their lightweight,high specific strength and specific modulus....Carbon nanotubes(CNTs)reinforced aluminum matrix composites(AMCs)show broad application prospects in the fields of aerospace and transportation because of their lightweight,high specific strength and specific modulus.A new alloying strategy in this study is proposed to regulate its weak intrinsic interface and uncontrollable interfacial reaction.Our results show that Si element could hinder the dissolution and diffusion of carbon atoms in Al matrix,inhibiting Al-CNTs interface reaction.Grain refinement and dislocation increment induced by the reinforcements promote the contributions to the strength of AMCs.The wettability and interface bonding of Al-CNTs could be effectively improved by Al/Si/CNTs composite interface,the formed discontinuous strong interface is advantageous to coordinate the plastic deformation of AMCs.Si particles can also firmly fix CNTs through pinning effect during deformation,which leads to a better load transfer.Therefore,the tensile strength of Al-5Si-0.5CNTs composite can be enhanced up to 391 MPa while maintaining an acceptable plasticity of 7.5%.It brings the strengthening effect of CNTs into full play in AMCs and achieves the strengthening effect of 1+1>2 under the comprehensive effect of grain refinement strengthening,dislocation strengthening,dispersion strengthening of Si particles and load transfer to CNTs。展开更多
Bismuth vanadate(BiVO_(4))is an excellent photoanode material for photoelectrochemical(PEC)water splitting system,possessing high theoretical photoelectrocatalytic conversion efficiency.However,the actual PEC activity...Bismuth vanadate(BiVO_(4))is an excellent photoanode material for photoelectrochemical(PEC)water splitting system,possessing high theoretical photoelectrocatalytic conversion efficiency.However,the actual PEC activity and stability of BiVO_(4)are faced with great challenges due to factors such as severe charge recombination and slow water oxidation kinetics at the interface.Therefore,various interface regulation strategies have been adopted to optimize the BiVO_(4)photoanode.This review provides an in-depth analysis for the mechanism of interface regulation strategies from the perspective of factors affecting the PEC performance of BiVO_(4)photoanodes.These interface regulation strategies improve the PEC performance of BiVO_(4)photoanode by promoting charge separation and transfer,accelerating interfacial reaction kinetics,and enhancing stability.The research on the interface regulation strategies of BiVO_(4)photoanode is of great significance for promoting the development of PEC water splitting technology.At the same time,it also has inspiration for providing new ideas and methods for designing and preparing efficient and stable catalytic materials.展开更多
Efficient photocatalysis and electrocatalysis in energy conversion have been important strategies to alleviate energy crises and environmental issues.In recent years,with the rapid development of emerging catalysts,si...Efficient photocatalysis and electrocatalysis in energy conversion have been important strategies to alleviate energy crises and environmental issues.In recent years,with the rapid development of emerging catalysts,significant progress has been made in photocatalysis for converting solar energy into chemical energy and electrocatalysis for converting electrical energy into chemical energy.However,their selectivity and efficiency of the products are poor.Rare earth(RE)can achieve atomic level fine regulation of catalysts and play an crucial role in optimizing catalyst performance by their unique electronic and orbital structures.However,there is a lack of systematic review on the atomic interface regulation mechanism of RE and their role in energy conversion processes.Single atom catalysts(SACs)provide clear active sites and 100%atomic utilization,which is conducive to exploring the regulatory mechanisms of RE.Therefore,this review mainly takes atomic level doped RE as an example to review and discuss the atomic interface regulation role of RE elements in energy conversion.Firstly,a brief introduction was given to the synthesis strategies that can effectively exert the atomic interface regulation effect of RE,with a focus on the atomic interface regulation mechanism of RE.Meanwhile,the regulatory mechanisms of RE atoms have been systematically summarized in various energy conversion applications.Finally,the challenges faced by RE in energy conversion,as well as future research directions and prospects,were pointed out.展开更多
Transition metal selenides have aroused great attention in recent years due to their high theoretical capacity.However,the huge volume fluctuation generated by conversion reaction during the charge/discharge process r...Transition metal selenides have aroused great attention in recent years due to their high theoretical capacity.However,the huge volume fluctuation generated by conversion reaction during the charge/discharge process results in the significant electrochemical performance reduction.Herein,the carbon-regulated copper(I)selenide(Cu_(2)Se@C)is designed to significantly promote the interface stability and ion diffusion for selenide electrodes.The systematic X-ray spectroscopies characterizations and density functional theory(DFT)simulations reveal that the Cu–Se–C bonding forming on the surface of Cu2Se not only improves the electronic conductivity of Cu_(2)Se@C but also retards the volume change during electrochemical cycling,playing a pivotal role in interface regulation.Consequently,the storage kinetics of Cu_(2)Se@C is mainly controlled by the capacitance process diverting from the ion diffusion-controlled process of Cu2Se.When employed this distinctive Cu_(2)Se@C as anode active material in Li coin cell configuration,the ultrahigh specific capacity of 810.3 mA·h·g^(−1)at 0.1 A·g^(−1)and the capacity retention of 83%after 1,500 cycles at 5 A·g^(−1)is achieved,implying the best Cu-based Li^(+)-storage capacity reported so far.This strategy of heterojunction combined with chemical bonding regulation opens up a potential way for the development of advanced electrodes for battery storage systems.展开更多
Rechargeable aqueous zinc-based batteries(RZBs)often suffer from poor cycling stability due to the instability of zinc deposition and etching processes.This work achieves dendrite-free zinc deposition with a smaller n...Rechargeable aqueous zinc-based batteries(RZBs)often suffer from poor cycling stability due to the instability of zinc deposition and etching processes.This work achieves dendrite-free zinc deposition with a smaller nucleation radius and rapid completion of the nucleation stage by a"triple regulation strategy"with trace chitosan oligosaccharide(COS)in ZnSO_(4)electrolyte(2 g L^(-1)COS),Theoretical and experimental results indicate that COS,with hydroxyl and amino functional groups,exhibits a high affinity for the(002)_(Zn)and(100)_(Zn)facets.Under the influence of a small amount of COS,the selective exposure of the(101)_(Zn)facet is facilitated.The extensively exposed(101)_(Zn)facet is protected by COS,which inhibits the occurrence of side reactions.Moreover,the presence of trace COS-02 changes the etching mode from three-dimensional(3D)to two-dimensional(2D),ensuring a uniform distribution of Zn^(2+)in the electric field during the deposition process.The unique 3D deposition and 2D etching mechanism induced by the COS additive result in exceptional cycling stability,exceeding 3800 h(1 mA cm^(-2))and 430 h(5 mA cm^(-2))in zinc symmetrical cells.Additionally,COS acts as a"molecular pillar"to stabilize VS_(2),enabling the Zn‖VS_(2)full cell to achieve 1000 stable cycles with 89.6%capacity retention and an average coulombic efficiency of 99.95%.This work reveals a novel multiple regulation mechanism by using trace COS in RZBs,and provides a new approach for the development of long-term stable RZBs with preferential exposure facets.展开更多
Aqueous zinc-iodine(Zn-I_(2))batteries show great potential as energy storage candidates due to their high-safety and low-cost,but confronts hydrogen evolution reaction(HER)and dendrite growth at anode side and polyio...Aqueous zinc-iodine(Zn-I_(2))batteries show great potential as energy storage candidates due to their high-safety and low-cost,but confronts hydrogen evolution reaction(HER)and dendrite growth at anode side and polyiodide shuttling at cathode side.Herein,"tennis racket"(TR)hydrogel electrolytes were prepared by the co-polymerization and co-blending of polyacrylamide(PAM),sodium lignosulfonate(SL),and sodium alginate(SA)to synchronously regulate cathode and anode of Zn-I_(2)batteries."Gridline structure"of TR can induce the uniform transportation of Zn^(2+)ions through the coordination effect to hinder HER and dendrite growth at anode side,as well as hit I_(3)^(-)ions as"tennis"via the strong repulsion force to avoid shuttle effect at cathode side.The synergistic effect of TR electrolyte endows Zn-Zn symmetric battery with high cycling stability over 4500 h and Zn-I_(2)cell with the stably cycling life of 15000 cycles at5 A g^(-1),outperforming the reported works.The practicability of TR electrolyte is verified by flexible Zn-I_(2)pouch battery.This work opens a route to synchronously regulate cathode and anode to enhance the electrochemical performance of Zn-I_(2)batteries.展开更多
The ultra-low permeability reservoir is regarded as an important energy source for oil and gas resource development and is attracting more and more attention.In this work,the active silica nanofuids were prepared by m...The ultra-low permeability reservoir is regarded as an important energy source for oil and gas resource development and is attracting more and more attention.In this work,the active silica nanofuids were prepared by modifed active silica nanoparticles and surfactant BSSB-12.The dispersion stability tests showed that the hydraulic radius of nanofuids was 58.59 nm and the zeta potential was−48.39 mV.The active nanofuids can simultaneously regulate liquid-liquid interface and solid-liquid interface.The nanofuids can reduce the oil/water interfacial tension(IFT)from 23.5 to 6.7 mN/m,and the oil/water/solid contact angle was altered from 42°to 145°.The spontaneous imbibition tests showed that the oil recovery of 0.1 wt%active nanofuids was 20.5%and 8.5%higher than that of 3 wt%NaCl solution and 0.1 wt%BSSB-12 solution.Finally,the efects of nanofuids on dynamic contact angle,dynamic interfacial tension and moduli were studied from the adsorption behavior of nanofuids at solid-liquid and liquid-liquid interface.The oil detaching and transporting are completed by synergistic efect of wettability alteration and interfacial tension reduction.The fndings of this study can help in better understanding of active nanofuids for EOR in ultra-low permeability reservoirs.展开更多
Precise control of the local environment and electronic state of the vip is an important method of controlling catalytic activity and reaction pathways.In this paper,vip Pd NPs were introduced into a series of hos...Precise control of the local environment and electronic state of the vip is an important method of controlling catalytic activity and reaction pathways.In this paper,vip Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce_(6)O_(6) or Zr_(6)O_(6)).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce_(6) clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99% and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pd^(δ+),which not only enhances the adsorption of H_(2) and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-vip interactions,and their correlation with catalytic performance.展开更多
Photocatalysis is a promising green approach for water purification.The diversity of water pH values is a key factor that restricts its practical application since pH affects the adsorption of organic molecules,the st...Photocatalysis is a promising green approach for water purification.The diversity of water pH values is a key factor that restricts its practical application since pH affects the adsorption of organic molecules,the stability of catalysts and photocatalytic performance.Here,we report a pH–independent,efficient and stable photocatalytic system with a liquid(water)–liquid(oil)–solid(semiconductor)(L–L–S)triphase interface microenvironment.The system is fabricated by coating a thin layer of silicon oil on the surface of ZnO nanowire arrays,a model chemically unstable semiconductor in both acidic and alkaline solutions.We show that the unique interface makes the dye adsorption pH independent and prevents the semiconductor from being corroded by strong acidic/alkaline solutions,leading to a stable and efficient photocatalytic reaction over a wide pH range(1—14).These findings reveal a promising path for the development of high-performance catalysis systems applicable in complex water environments.展开更多
Single-atom site catalysts(SACs)have made great achievements due to their nearly 100%atomic utilization and uniform active sites.Regulating the surrounding environment of active sites,including electron structure and ...Single-atom site catalysts(SACs)have made great achievements due to their nearly 100%atomic utilization and uniform active sites.Regulating the surrounding environment of active sites,including electron structure and coordination environment via atom-level interface regulation,to design and construct an advanced SACs is of great significance for boosting electrocatalytic reactions.In this review,we systemically summarized the fundamental understandings and intrinsic mechanisms of SACs for electrocatalytic applications based on the interface site regulations.We elaborated the several different regulation strategies of SACs to demonstrate their ascendancy in electrocatalytic applications.Firstly,the interfacial electronic interaction was presented to reveal the electron transfer behavior of active sites.Secondly,the different coordination structures of metal active center coordinated with two or three non-metal elements were also summarized.In addition,other atom-level interfaces of SACs,including metal atom–atom interface,metal atom-X-atom interface(X:non-metal element),metal atom-particle interface,were highlighted and the corresponding promoting effect towards electrocatalysis was disclosed.Finally,we outlooked the limitations,perspectives and challenges of SACs based on atomic interface regulation.展开更多
Silver chalcogenides(Ag_(2)E;E=S,Se,or Te)quantum dots(QDs)have emerged as promising candidates for near-infrared(NIR)applications.However,their narrow bandgap and small exciton Bohr radius render the optical properti...Silver chalcogenides(Ag_(2)E;E=S,Se,or Te)quantum dots(QDs)have emerged as promising candidates for near-infrared(NIR)applications.However,their narrow bandgap and small exciton Bohr radius render the optical properties of Ag_(2)E QDs highly sensitive to surface and size variations.Moreover,the propensity for the formation of silver impurities and their low solubility product constants pose challenges in their controllable synthesis.Recent advancements have deepened our understanding of the relationship between the multi-hierarchical structure of Ag_(2)E QDs and their optical properties.Through rational design and precise structural regulation,the performance of Ag_(2)E QDs has been significantly enhanced across various applications.This review provides a comprehensive overview of historical and current progress in the synthesis and structural regulation of Ag_(2)E QDs,encompassing aspects such as size control,crystal structure engineering,and surface/interface engineering.Additionally,it discusses outstanding challenges and potential opportunities in this field.The aim of this review is to promote the custom synthesis of Ag_(2)E QDs for applications in biological imaging,and optoelectronics applications.展开更多
Solar-driven CO_(2)conversion into value-added chemical provides an attractive strategy for sustainable development.However,the enhanced CO_(2)photoreduction performance with target product selectivity remains a major...Solar-driven CO_(2)conversion into value-added chemical provides an attractive strategy for sustainable development.However,the enhanced CO_(2)photoreduction performance with target product selectivity remains a major challenge.Here,we develop a novel strategy involving Cu_(2)O nanoparticles in situ grown on the surface of ZIF-67-derived Co@C-N nanocages(CC)to create abundant active sites and appropriate heterointerfaces.A remarkable CO selectivity of 95.7%with a yield of 117.39μmol g-1h-1and an apparent quantum efficiency as high as 1.88%at 420 nm was obtained over CC-60 catalyst in pure water,which was 87.6 times higher than that of pure Cu_(2)O.Theoretical calculations and experiments indicated that Co@C-N nanocages as charge mediator not only rapidly trap photogenerated electrons to promote charge separation efficiency,but also regulate the d-band center of Cu atoms to move to the Fermi energy level,thereby optimizing the reaction kinetics to facilitate the highly selective conversion of the key intermediate*CO desorption to CO.展开更多
Hydrogen fuel cells with high energy conversion efficiency and zero carbon emissions play a critical role in addressing energy crises and environmental pollution,when the hydrogen is derived from renewable energy-powe...Hydrogen fuel cells with high energy conversion efficiency and zero carbon emissions play a critical role in addressing energy crises and environmental pollution,when the hydrogen is derived from renewable energy-powered water electrolysis.The core of the reaction lies in the catalytic reaction interface.At this interface,the complex interactions among catalysts,aqueous environments,ion species,and ionomers directly determine the efficiency of the catalytic reaction.This review systematically summarized four key interfacial influencing factors,including adsorption behavior of catalysts,interfacial water dynamics,ion modification,and ionomer-electrode interactions.It provided an in-depth summary of key regulation strategies such as catalyst engineering,interfacial water structure optimization,ionic group functionalization,and interface reinforcement.Furthermore,future development directions are proposed,focusing on in-situ characterization,multiphase interface engineering,durability enhancement of non-precious metal catalysts,and machine learning-driven multiscale modeling,aiming to establish fuel cells as a cornerstone of sustainable energy systems.展开更多
Red mud is a kind of industrial waste residue produced in the process of alumina production,which has strong suspension and is difficult to precipitate and filter.This study compared the effects of 4 kinds of filter a...Red mud is a kind of industrial waste residue produced in the process of alumina production,which has strong suspension and is difficult to precipitate and filter.This study compared the effects of 4 kinds of filter aids,including CaCl2,polymerized ferrous sulfate(PFS),steel slag(SS),and Portland cement(PC),on the filtration rate,filter cake moisture content,and Na2O content of red mud slurry.At a dosage of 10 g·L^(-1),the filtration effects were in the following order:PFS>CaCl_(2)>SS>PC.Under the combination of 5 g·L^(-1) SS and 5 g·L^(-1) PC,the better filtration effect was achieved with a filtration time of 205.17 s,which was reduced by 58.52%compared to the original red mud.The combined use of SS and PC exhibits better advantages in terms of cost and filtration effect.This study provides a data foundation for the rapid filtration of red mud slurry.The use of SS and PC as filter aids for red mud holds broad application pro-spects.展开更多
Constructing hetero-structured catalyst is promising but still challenging to achieve overall water splitting for hydrogen production with high efficiency.Herein,we developed a sulfide-based MoS_(2)/Co_(l-x)S@C hetero...Constructing hetero-structured catalyst is promising but still challenging to achieve overall water splitting for hydrogen production with high efficiency.Herein,we developed a sulfide-based MoS_(2)/Co_(l-x)S@C hetero-structure for highly efficient electrochemical hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The carbon derived from the filter paper acts as a conducting carrier to ensure adequate exposure of the active sites guaranteed with improved catalytic stability.The unique hierarchical nano-sheets facilitate the charge and ion transfer by shortening the diffusion path during electro-catalysis.Meanwhile,the robust hetero-interfaces in MoS_(2)/Co_(1-x)S@C can expose rich electrochemical active sites and facilitate the charge transfer,which further cooperates synergistically toward electro-catalytic reactions.Consequently,the optimal MoS_(2)/Co_(1-x)S@C hetero-structures present small over-potentials toward HER(135 mV@10 mA·cm^(-2))and OER(230 mV@10 mA·cm^(-2)).The MoS_(2)/Co_(1-x)S@C electrolyzer requires an ultralow voltage of 1.6 V at the current density of 10 mA·cm^(-2)with excellent durability,outperforming the state-of-the-art electro-catalysts.This work sheds light on the design of the hetero-structured catalysts with interfacial engineering toward large-scale water splitting.展开更多
基金supported by the National Natural Science Foundation of China(22179053,22279046)Natural Science Excellent Youth Foundation of Jiangsu Provincial(BK20220112)+1 种基金Special Foundation for Carbon Peak Carbon Neutralization Technology Innovation Program of Jiangsu Province(BE2022026-2)JSPS KAKENHI(20K15385,20H02817,and 24H00486)。
文摘Organic molecule passivation of perovskite surfaces has emerged as a promising strategy for efficient and durable perovskite solar cells(PSCs).While many materials have been reported,the optimization of molecular structure for the best passivation effect remains of significant interest but lacks sufficient study.In this work,we designed and synthesized three novel donor–acceptor-donor(D-A-D)type conjugated organic small molecules with varying alkyl chain lengths to regulate the interface between perovskite and Spiro-OMeTAD.Among them,the OSIT molecule,which features an n-octyl side chain of optimal length,demonstrated a balanced interfacial contact and interaction with the perovskite surface.Beyond the passivation effect of the electron-rich C=O group on undercoordinated Pb2+defects,OSIT optimizes energy level alignment and improves charge extraction by acting as an efficient hole transport channel.As a result,PSCs with OSIT interfacial layer achieved an exceptional efficiency of 25.48%and a high open-circuit voltage of 1.18 V.Furthermore,the durability of unencapsulated devices was significantly enhanced under various environmental conditions,maintaining 93.7%of their initial efficiency after 1000 h of maximum power point tracking in a nitrogen atmosphere.This study provides valuable insights into the rational design of D-A-D type materials for effective interface modification in PSCs.
基金the financial support from the National Natural Science Foundation of China(62274132,62204189,62274126)the Postdoctoral Fellowship Program of CPSF(GZC20241301)+1 种基金Fundamental Research Funds for the Central Universities(ZYTS25221)the National Key R&D Program of China(2022YFB3605402,2021YFF0500501)。
文摘All-inorganic perovskite materials exhibit exceptional thermal stability and promising candidates for tandem devices,while their application is still in the initial stage.Here,a metal halide doping strategy was implemented to enhance device performance and stability for inverted CsPbI_(3)perovskite solar cells(PSCs),which are ideal for integration into perovskite/silicon tandem solar cells.The lanthanide compound terbium chloride(TbCl_(3))was employed to improve buried interface between[4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl]phosphonic acid(Me-4PACz)and perovskite layer,thereby enhancing the crystallinity of CsPbI_(3)films and passivating non-radiative recombination defects.Thus,the inverted CsPbI_(3)PSCs achieved an efficiency of 18.68%and demonstrated excellent stability against water and oxygen.Meanwhile,remarkable efficiencies of 29.40%and 25.44%were,respectively,achieved in four-terminal(4T)and two-terminal(2T)perovskite/silicon mechanically tandem devices,which are higher efficiencies among reported all-inorganic perovskite-based tandem solar cells.This study presents a novel approach for fabricating highly efficient and stable inverted all-inorganic PSCs and perovskite/silicon tandem solar cells.
基金supported by the National Natural Science Foundation of China(Nos.52201165 and 51871180)the Guangdong Basic and Applied Basic Research Foundation(No.2021A1515111163)+2 种基金the Guangdong Introducing Innovative and Enterpreneurial Teams(No.2016ZT06G025)the National Key R&D Program of China(No.2021YFB3701203)supported by the Doctoral Teacher Starting Fund of Xi’an University of Technology(Nos.101-451121007 and 101-451121008).
文摘Carbon nanotubes(CNTs)reinforced aluminum matrix composites(AMCs)show broad application prospects in the fields of aerospace and transportation because of their lightweight,high specific strength and specific modulus.A new alloying strategy in this study is proposed to regulate its weak intrinsic interface and uncontrollable interfacial reaction.Our results show that Si element could hinder the dissolution and diffusion of carbon atoms in Al matrix,inhibiting Al-CNTs interface reaction.Grain refinement and dislocation increment induced by the reinforcements promote the contributions to the strength of AMCs.The wettability and interface bonding of Al-CNTs could be effectively improved by Al/Si/CNTs composite interface,the formed discontinuous strong interface is advantageous to coordinate the plastic deformation of AMCs.Si particles can also firmly fix CNTs through pinning effect during deformation,which leads to a better load transfer.Therefore,the tensile strength of Al-5Si-0.5CNTs composite can be enhanced up to 391 MPa while maintaining an acceptable plasticity of 7.5%.It brings the strengthening effect of CNTs into full play in AMCs and achieves the strengthening effect of 1+1>2 under the comprehensive effect of grain refinement strengthening,dislocation strengthening,dispersion strengthening of Si particles and load transfer to CNTs。
基金supported by the National Natural Science Foundation of China(52202261)Outstanding Youth Foundation of Shandong Province,China(ZR2019JQ 14)Taishan Scholar Young Talent Program(tsqn201909114).
文摘Bismuth vanadate(BiVO_(4))is an excellent photoanode material for photoelectrochemical(PEC)water splitting system,possessing high theoretical photoelectrocatalytic conversion efficiency.However,the actual PEC activity and stability of BiVO_(4)are faced with great challenges due to factors such as severe charge recombination and slow water oxidation kinetics at the interface.Therefore,various interface regulation strategies have been adopted to optimize the BiVO_(4)photoanode.This review provides an in-depth analysis for the mechanism of interface regulation strategies from the perspective of factors affecting the PEC performance of BiVO_(4)photoanodes.These interface regulation strategies improve the PEC performance of BiVO_(4)photoanode by promoting charge separation and transfer,accelerating interfacial reaction kinetics,and enhancing stability.The research on the interface regulation strategies of BiVO_(4)photoanode is of great significance for promoting the development of PEC water splitting technology.At the same time,it also has inspiration for providing new ideas and methods for designing and preparing efficient and stable catalytic materials.
基金support from the National Natural Science Foundation of China(Nos.21875021,22075024)the Beijing Natural Science Foundation(No.2212018).
文摘Efficient photocatalysis and electrocatalysis in energy conversion have been important strategies to alleviate energy crises and environmental issues.In recent years,with the rapid development of emerging catalysts,significant progress has been made in photocatalysis for converting solar energy into chemical energy and electrocatalysis for converting electrical energy into chemical energy.However,their selectivity and efficiency of the products are poor.Rare earth(RE)can achieve atomic level fine regulation of catalysts and play an crucial role in optimizing catalyst performance by their unique electronic and orbital structures.However,there is a lack of systematic review on the atomic interface regulation mechanism of RE and their role in energy conversion processes.Single atom catalysts(SACs)provide clear active sites and 100%atomic utilization,which is conducive to exploring the regulatory mechanisms of RE.Therefore,this review mainly takes atomic level doped RE as an example to review and discuss the atomic interface regulation role of RE elements in energy conversion.Firstly,a brief introduction was given to the synthesis strategies that can effectively exert the atomic interface regulation effect of RE,with a focus on the atomic interface regulation mechanism of RE.Meanwhile,the regulatory mechanisms of RE atoms have been systematically summarized in various energy conversion applications.Finally,the challenges faced by RE in energy conversion,as well as future research directions and prospects,were pointed out.
基金financially supported in part by the National Key Research and Development Program of China(No.2020YFA0405800)the National Natural Science Foundation of China(NSFC,Nos.U1932201 and U2032113)+4 种基金Youth Innovation Promotion Association of Chinese Academy of Sciences(CAS)(No.2022457)CAS Collaborative Innovation Program of Hefei Science Center(No.2020HSC-CIP002)CAS International Partnership Program(No.211134KYSB20190063)the Fundamental Research Funds for the Central Universities(No.WK2060000039)L.S.acknowledges the support from the Institute of Energy,Hefei Comprehensive National Science Center,University Synergy Innovation Program of Anhui Province(No.GXXT-2020-002).
文摘Transition metal selenides have aroused great attention in recent years due to their high theoretical capacity.However,the huge volume fluctuation generated by conversion reaction during the charge/discharge process results in the significant electrochemical performance reduction.Herein,the carbon-regulated copper(I)selenide(Cu_(2)Se@C)is designed to significantly promote the interface stability and ion diffusion for selenide electrodes.The systematic X-ray spectroscopies characterizations and density functional theory(DFT)simulations reveal that the Cu–Se–C bonding forming on the surface of Cu2Se not only improves the electronic conductivity of Cu_(2)Se@C but also retards the volume change during electrochemical cycling,playing a pivotal role in interface regulation.Consequently,the storage kinetics of Cu_(2)Se@C is mainly controlled by the capacitance process diverting from the ion diffusion-controlled process of Cu2Se.When employed this distinctive Cu_(2)Se@C as anode active material in Li coin cell configuration,the ultrahigh specific capacity of 810.3 mA·h·g^(−1)at 0.1 A·g^(−1)and the capacity retention of 83%after 1,500 cycles at 5 A·g^(−1)is achieved,implying the best Cu-based Li^(+)-storage capacity reported so far.This strategy of heterojunction combined with chemical bonding regulation opens up a potential way for the development of advanced electrodes for battery storage systems.
基金supported by the National Natural Science Foundation of China(52161145503)。
文摘Rechargeable aqueous zinc-based batteries(RZBs)often suffer from poor cycling stability due to the instability of zinc deposition and etching processes.This work achieves dendrite-free zinc deposition with a smaller nucleation radius and rapid completion of the nucleation stage by a"triple regulation strategy"with trace chitosan oligosaccharide(COS)in ZnSO_(4)electrolyte(2 g L^(-1)COS),Theoretical and experimental results indicate that COS,with hydroxyl and amino functional groups,exhibits a high affinity for the(002)_(Zn)and(100)_(Zn)facets.Under the influence of a small amount of COS,the selective exposure of the(101)_(Zn)facet is facilitated.The extensively exposed(101)_(Zn)facet is protected by COS,which inhibits the occurrence of side reactions.Moreover,the presence of trace COS-02 changes the etching mode from three-dimensional(3D)to two-dimensional(2D),ensuring a uniform distribution of Zn^(2+)in the electric field during the deposition process.The unique 3D deposition and 2D etching mechanism induced by the COS additive result in exceptional cycling stability,exceeding 3800 h(1 mA cm^(-2))and 430 h(5 mA cm^(-2))in zinc symmetrical cells.Additionally,COS acts as a"molecular pillar"to stabilize VS_(2),enabling the Zn‖VS_(2)full cell to achieve 1000 stable cycles with 89.6%capacity retention and an average coulombic efficiency of 99.95%.This work reveals a novel multiple regulation mechanism by using trace COS in RZBs,and provides a new approach for the development of long-term stable RZBs with preferential exposure facets.
基金financially supported by the Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy(E411060316)the NSFC-CONICFT Joint Project(51961125207)+1 种基金the Special Fund(2024)of Basic Scientific Research Project at Undergraduate University in Liaoning Province(LJ212410152056)the Foundation(GZKF202301)of State Key Laboratory of Biobased Material and Green Papermaking,Qilu University of Technology,Shandong Academy of Sciences。
文摘Aqueous zinc-iodine(Zn-I_(2))batteries show great potential as energy storage candidates due to their high-safety and low-cost,but confronts hydrogen evolution reaction(HER)and dendrite growth at anode side and polyiodide shuttling at cathode side.Herein,"tennis racket"(TR)hydrogel electrolytes were prepared by the co-polymerization and co-blending of polyacrylamide(PAM),sodium lignosulfonate(SL),and sodium alginate(SA)to synchronously regulate cathode and anode of Zn-I_(2)batteries."Gridline structure"of TR can induce the uniform transportation of Zn^(2+)ions through the coordination effect to hinder HER and dendrite growth at anode side,as well as hit I_(3)^(-)ions as"tennis"via the strong repulsion force to avoid shuttle effect at cathode side.The synergistic effect of TR electrolyte endows Zn-Zn symmetric battery with high cycling stability over 4500 h and Zn-I_(2)cell with the stably cycling life of 15000 cycles at5 A g^(-1),outperforming the reported works.The practicability of TR electrolyte is verified by flexible Zn-I_(2)pouch battery.This work opens a route to synchronously regulate cathode and anode to enhance the electrochemical performance of Zn-I_(2)batteries.
基金This work was fnancially supported by National Natural Science Foundation of China(52074333,51874337)Taishan Scholar Foundation of Shandong Province(tspd20161004)Fundamental Research Funds for the Central Universities(19CX07001A).
文摘The ultra-low permeability reservoir is regarded as an important energy source for oil and gas resource development and is attracting more and more attention.In this work,the active silica nanofuids were prepared by modifed active silica nanoparticles and surfactant BSSB-12.The dispersion stability tests showed that the hydraulic radius of nanofuids was 58.59 nm and the zeta potential was−48.39 mV.The active nanofuids can simultaneously regulate liquid-liquid interface and solid-liquid interface.The nanofuids can reduce the oil/water interfacial tension(IFT)from 23.5 to 6.7 mN/m,and the oil/water/solid contact angle was altered from 42°to 145°.The spontaneous imbibition tests showed that the oil recovery of 0.1 wt%active nanofuids was 20.5%and 8.5%higher than that of 3 wt%NaCl solution and 0.1 wt%BSSB-12 solution.Finally,the efects of nanofuids on dynamic contact angle,dynamic interfacial tension and moduli were studied from the adsorption behavior of nanofuids at solid-liquid and liquid-liquid interface.The oil detaching and transporting are completed by synergistic efect of wettability alteration and interfacial tension reduction.The fndings of this study can help in better understanding of active nanofuids for EOR in ultra-low permeability reservoirs.
文摘Precise control of the local environment and electronic state of the vip is an important method of controlling catalytic activity and reaction pathways.In this paper,vip Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce_(6)O_(6) or Zr_(6)O_(6)).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce_(6) clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99% and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pd^(δ+),which not only enhances the adsorption of H_(2) and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-vip interactions,and their correlation with catalytic performance.
基金supported by the National Key R&D Program of China(2019YFA0709200)the National Natural Science Foundation of China(21988102,51772198,21975171)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Photocatalysis is a promising green approach for water purification.The diversity of water pH values is a key factor that restricts its practical application since pH affects the adsorption of organic molecules,the stability of catalysts and photocatalytic performance.Here,we report a pH–independent,efficient and stable photocatalytic system with a liquid(water)–liquid(oil)–solid(semiconductor)(L–L–S)triphase interface microenvironment.The system is fabricated by coating a thin layer of silicon oil on the surface of ZnO nanowire arrays,a model chemically unstable semiconductor in both acidic and alkaline solutions.We show that the unique interface makes the dye adsorption pH independent and prevents the semiconductor from being corroded by strong acidic/alkaline solutions,leading to a stable and efficient photocatalytic reaction over a wide pH range(1—14).These findings reveal a promising path for the development of high-performance catalysis systems applicable in complex water environments.
基金supported by the National Key R&D Program of China(2018YFA0702003)the National Natural Science Foundation of China(21890383,21871159)the Science and Technology Key Project of Guangdong Province of China(2020B010188002)。
文摘Single-atom site catalysts(SACs)have made great achievements due to their nearly 100%atomic utilization and uniform active sites.Regulating the surrounding environment of active sites,including electron structure and coordination environment via atom-level interface regulation,to design and construct an advanced SACs is of great significance for boosting electrocatalytic reactions.In this review,we systemically summarized the fundamental understandings and intrinsic mechanisms of SACs for electrocatalytic applications based on the interface site regulations.We elaborated the several different regulation strategies of SACs to demonstrate their ascendancy in electrocatalytic applications.Firstly,the interfacial electronic interaction was presented to reveal the electron transfer behavior of active sites.Secondly,the different coordination structures of metal active center coordinated with two or three non-metal elements were also summarized.In addition,other atom-level interfaces of SACs,including metal atom–atom interface,metal atom-X-atom interface(X:non-metal element),metal atom-particle interface,were highlighted and the corresponding promoting effect towards electrocatalysis was disclosed.Finally,we outlooked the limitations,perspectives and challenges of SACs based on atomic interface regulation.
基金supported by the National Natural Science Foundation of China(Nos.22293030 and 22293032)the China Postdoctoral Science Foundation(No.2022M721697).
文摘Silver chalcogenides(Ag_(2)E;E=S,Se,or Te)quantum dots(QDs)have emerged as promising candidates for near-infrared(NIR)applications.However,their narrow bandgap and small exciton Bohr radius render the optical properties of Ag_(2)E QDs highly sensitive to surface and size variations.Moreover,the propensity for the formation of silver impurities and their low solubility product constants pose challenges in their controllable synthesis.Recent advancements have deepened our understanding of the relationship between the multi-hierarchical structure of Ag_(2)E QDs and their optical properties.Through rational design and precise structural regulation,the performance of Ag_(2)E QDs has been significantly enhanced across various applications.This review provides a comprehensive overview of historical and current progress in the synthesis and structural regulation of Ag_(2)E QDs,encompassing aspects such as size control,crystal structure engineering,and surface/interface engineering.Additionally,it discusses outstanding challenges and potential opportunities in this field.The aim of this review is to promote the custom synthesis of Ag_(2)E QDs for applications in biological imaging,and optoelectronics applications.
基金supported by the National Natural Science Foundation of China(22372013 and 22278042)Changzhou Leading Innovative Talents Introduction and Cultivation(CQ20230108)。
文摘Solar-driven CO_(2)conversion into value-added chemical provides an attractive strategy for sustainable development.However,the enhanced CO_(2)photoreduction performance with target product selectivity remains a major challenge.Here,we develop a novel strategy involving Cu_(2)O nanoparticles in situ grown on the surface of ZIF-67-derived Co@C-N nanocages(CC)to create abundant active sites and appropriate heterointerfaces.A remarkable CO selectivity of 95.7%with a yield of 117.39μmol g-1h-1and an apparent quantum efficiency as high as 1.88%at 420 nm was obtained over CC-60 catalyst in pure water,which was 87.6 times higher than that of pure Cu_(2)O.Theoretical calculations and experiments indicated that Co@C-N nanocages as charge mediator not only rapidly trap photogenerated electrons to promote charge separation efficiency,but also regulate the d-band center of Cu atoms to move to the Fermi energy level,thereby optimizing the reaction kinetics to facilitate the highly selective conversion of the key intermediate*CO desorption to CO.
基金supported by the National Natural Science Foundation of China(52021004 and 22279082)Sichuan Science and Technology Program(2025YFHZ0056).
文摘Hydrogen fuel cells with high energy conversion efficiency and zero carbon emissions play a critical role in addressing energy crises and environmental pollution,when the hydrogen is derived from renewable energy-powered water electrolysis.The core of the reaction lies in the catalytic reaction interface.At this interface,the complex interactions among catalysts,aqueous environments,ion species,and ionomers directly determine the efficiency of the catalytic reaction.This review systematically summarized four key interfacial influencing factors,including adsorption behavior of catalysts,interfacial water dynamics,ion modification,and ionomer-electrode interactions.It provided an in-depth summary of key regulation strategies such as catalyst engineering,interfacial water structure optimization,ionic group functionalization,and interface reinforcement.Furthermore,future development directions are proposed,focusing on in-situ characterization,multiphase interface engineering,durability enhancement of non-precious metal catalysts,and machine learning-driven multiscale modeling,aiming to establish fuel cells as a cornerstone of sustainable energy systems.
基金supported by the Science and Technology Innovation Program of Hunan Province,China(No.2023RC3053)the National Key Research and Development Program of China(No.2023YFC3904201)the National Natural Science Foundation of China(No.52004343).
文摘Red mud is a kind of industrial waste residue produced in the process of alumina production,which has strong suspension and is difficult to precipitate and filter.This study compared the effects of 4 kinds of filter aids,including CaCl2,polymerized ferrous sulfate(PFS),steel slag(SS),and Portland cement(PC),on the filtration rate,filter cake moisture content,and Na2O content of red mud slurry.At a dosage of 10 g·L^(-1),the filtration effects were in the following order:PFS>CaCl_(2)>SS>PC.Under the combination of 5 g·L^(-1) SS and 5 g·L^(-1) PC,the better filtration effect was achieved with a filtration time of 205.17 s,which was reduced by 58.52%compared to the original red mud.The combined use of SS and PC exhibits better advantages in terms of cost and filtration effect.This study provides a data foundation for the rapid filtration of red mud slurry.The use of SS and PC as filter aids for red mud holds broad application pro-spects.
基金supported by the National Natural Science Foundation of China(51871119,22075141,and 22101132)Scientific and Technological Innovation Special Fund for Carbon Peak and Carbon Neutrality of Jiangsu Province(BK20220039)+3 种基金Jiangsu Provincial Founds for Natural Science Foundation(BK20180015 and BK20210311)China Postdoctoral Science Foundation(2021M691561 and 2021T140319)Jiangsu Postdoctoral Research Fund(2021K547C)the Fundamental Research Funds for the Central Universities(kfjj20180605)。
文摘Constructing hetero-structured catalyst is promising but still challenging to achieve overall water splitting for hydrogen production with high efficiency.Herein,we developed a sulfide-based MoS_(2)/Co_(l-x)S@C hetero-structure for highly efficient electrochemical hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).The carbon derived from the filter paper acts as a conducting carrier to ensure adequate exposure of the active sites guaranteed with improved catalytic stability.The unique hierarchical nano-sheets facilitate the charge and ion transfer by shortening the diffusion path during electro-catalysis.Meanwhile,the robust hetero-interfaces in MoS_(2)/Co_(1-x)S@C can expose rich electrochemical active sites and facilitate the charge transfer,which further cooperates synergistically toward electro-catalytic reactions.Consequently,the optimal MoS_(2)/Co_(1-x)S@C hetero-structures present small over-potentials toward HER(135 mV@10 mA·cm^(-2))and OER(230 mV@10 mA·cm^(-2)).The MoS_(2)/Co_(1-x)S@C electrolyzer requires an ultralow voltage of 1.6 V at the current density of 10 mA·cm^(-2)with excellent durability,outperforming the state-of-the-art electro-catalysts.This work sheds light on the design of the hetero-structured catalysts with interfacial engineering toward large-scale water splitting.
