Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains...Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.展开更多
Spatial confinement of block copolymers can induce frustrations,which can further be utilized to regulate self-assembled structures,thus providing an efficient route for fabricating novel structures.We studied the sel...Spatial confinement of block copolymers can induce frustrations,which can further be utilized to regulate self-assembled structures,thus providing an efficient route for fabricating novel structures.We studied the self-assembly of AB di-block copolymers(di-BCPs)confined in Janus spherical nanocavities using simulations,and explained the structure formation mechanisms.In the case of a strongly selective cavity wall,all the lamella-forming,gyroid-forming,and cylinder-forming di-BCPs can form interfacial frustration-induced Janus concentric perforated lamellar nanoparticles,whose outermost is a Janus spherical shell and the internal is a sphere with concentric perforated lamellar structure.In particular,Janus concentric perforated lamellar nanoparticles with holes distributed only near the equatorial plane were obtained in both lamella-forming and gyroid-forming di-BCPs,directly reflecting the effect of interfacial frustration.The minority-block domain of the cylider-forming di-BCPs may form hemispherical perforated lamellar structures with holes distributed in parallel layers with a specific orientation.For symmetric di-BCPs,both the A and B domains in each nanoparticle are continuous,interchangeable,and have rotational symmetry.While for gyroid-forming and cylinder-forming di-BCPs,only the majority-block domains are continuous in each nanoparticle,and holes in the minority-block domains usually have rotational symmetry.In the case of a weakly selective cavity wall,the inhomogeneity of the cavity wall results in structures having a specific orientation(such as flower-like and branched structures in gyroid-forming and cylinder-forming di-BCPs)and a perforated wetting layer with uniformly distributed holes.The novel nanoparticles obtained may have potential applications in nanotechnology as functional nanostructures or nanoparticles.展开更多
The NiOx,due to its excellent semiconductor properties,ease of large-area deposition,and tunable optoelectronic characteristics,shows great potential in industrial large-area perovskite technologies.However,NiO_(x)-ba...The NiOx,due to its excellent semiconductor properties,ease of large-area deposition,and tunable optoelectronic characteristics,shows great potential in industrial large-area perovskite technologies.However,NiO_(x)-based perovskite solar cells(PSCs)are limited by interfacial photocatalytic chemical reactions and energy level mismatch.Thus,phosphate-based self-assembled monolayers(SAMs)have been widely developed for delicate interfacial modification;however,they suffer from severe issues such as self-aggregation and high cost.Herein,a low-cost carboxylate-based SAM(pyrenebutyric acid,PyBA)was used to modify NiO_(x),achieving an improved surface chemical environment and interfacial properties,such as an increased Ni^(3+)/Ni2^(+)ratio,a reduced proportion of high-valence Ni^(≥3+),and better-aligned hole transport interface energy level.The introduction of PyBA also results in larger grain size,higher uniformity,and enhanced photoluminescence(PL)from the bottom of the perovskite,yielding a significant increase in efficiency from an initial 22.48%to 25.14%,while increasing the open-circuit voltage(VOC)from 1.077 to 1.192 V.Additionally,a perovskite module with an aperture area of 21 cm^(2)achieved an efficiency of 22.28%,demonstrating the excellent scalability of the PyBA treatment.Moreover,the well-modified buried interface combined with the chemical inertness and structural rigidity of pyrene ensures excellent ultraviolet(UV)stability(the target module maintained 92%of the initial efficiency after 200 h and the control device only retained 40%).展开更多
The interfacial property of carbon fiber(CF)reinforced composites is crucial to facilitate the application of high-strength composites.Utilizing the electrostatic and hydrogen bond properties of diazo resin,carbon nan...The interfacial property of carbon fiber(CF)reinforced composites is crucial to facilitate the application of high-strength composites.Utilizing the electrostatic and hydrogen bond properties of diazo resin,carbon nanotubes(CNTs)and graphene oxide(GO)could be quickly grafted onto the surface of the CF via the layer-by-layer self-assembly technique.The results showed that CNTs and GO were uniformly coated onto the CF surface,and the chemical activity and roughness of the modified CF surface were improved signif-icantly.The modified CF surface can significantly augment the interaction between the epoxy resin and the fiber.Remarkably,due to the good interfacial property,the impact performance of the composites re-inforced with the nanomaterial-modified CF was improved obviously.In addition,the interface properties of the composites are studied in depth.This method is expected to achieve rapid surface modification of carbon fiber.展开更多
The chiral self-assembly of functional molecules,polymers and clus-ters into nanoscale objects with well-defined ordering,asymmetry and in some cases out-of-equilibrium characteristics is an important strategy to fabr...The chiral self-assembly of functional molecules,polymers and clus-ters into nanoscale objects with well-defined ordering,asymmetry and in some cases out-of-equilibrium characteristics is an important strategy to fabricate novel materials[1],which might address key challenges at the heart of energy,environmental and biomedical applications.In recent years,subsequent utilization of these nanoscale units as new building blocks to fabricate advanced structures and realize more complex func-tions like those in the biology systems has aroused interests.These at-tempts are originated from the concept of molecular nanotechnology but have gone beyond its boundaries towards the breakthroughs of self-assembled machines,advanced nanoarchitectonics and molecular nanotopology[2,3].展开更多
Wettability transition is a significant responsive mechanism which is widely applied to construct smart materials and systems.The broad-spectrum responsiveness of the wettability transition makes it a promising way to...Wettability transition is a significant responsive mechanism which is widely applied to construct smart materials and systems.The broad-spectrum responsiveness of the wettability transition makes it a promising way to expand innovative applications.Here,we develop a track-guided self-transportation system mediated by sequential wettability transition accompanied with capillary transportation.Alkaline fuel is loaded into polydimethylsiloxane(PDMS)cuboid to trigger the wettability transition of distributed superhydrophobic tracks laid in shallow water.After the wettability transition,the induced capillary force can propel the repetitive track-to-track transportation of PDMS.Importantly,the spacing between adjacent tracks is rationally designed based on multiple factors including threshold of wettability transition,diffusion kinetics and capillary interaction.Furthermore,the track-guided transportation system is applied to realize directed self-assembly of multiple PDMS building blocks for designated configuration,which increases the complexity and intelligence of self-assembly systems.展开更多
The utilization of solar-driven interfacial evaporation technology is highly important in addressing the energy crisis and water scarcity,primarily because of its affordability and minimal energy usage.Enhancing the p...The utilization of solar-driven interfacial evaporation technology is highly important in addressing the energy crisis and water scarcity,primarily because of its affordability and minimal energy usage.Enhancing the performance of solar energy evaporation and minimizing material degradation during application can be achieved through the design of novel photothermal materials.In solar interfacial evaporation,photothermal materials exhibit a wide range of additional characteristics,but a systematic overview is lacking.This paper encompasses an examination of various categories and principles pertaining to photothermal materials,as well as the structural design considerations for salt-resistant materials.Additionally,we discuss the versatile uses of this appealing technology in different sectors related to energy and the environment.Furthermore,potential solutions to enhance the durability of photothermal materials are also highlighted,such as the rational design of micro/nano-structures,the use of adhesives,the addition of anti-corrosion coatings,and the preparation of self-healing surfaces.The objective of this review is to offer a viable resolution for the logical creation of high-performance photothermal substances,presenting a guide for the forthcoming advancement of solar evaporation technology.展开更多
NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy leve...NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.展开更多
Revealing the structure evolution of interfacial active species during a dynamic catalytic process is a challenging but pivotal issue for the rational design of high-performance catalysts.Here,we successfully prepare ...Revealing the structure evolution of interfacial active species during a dynamic catalytic process is a challenging but pivotal issue for the rational design of high-performance catalysts.Here,we successfully prepare sub-nanometric Pt clusters(~0.8 nm)encapsulated within the defects of CeO_(2)nanorods via an in-situ defect engineering methodology.The as-prepared Pt@d-CeO_(2)catalyst significantly boosts the activity and stability in the water-gas shift(WGS)reaction compared to other analogs.Based on controlled experiments and complementary(in-situ)spectroscopic studies,a reversible encapsulation induced by active site transformation between the Pt^(2+)-terminal hydroxyl and Pt^(δ+)-O vacancy species at the interface is revealed,which enables to evoke the enhanced performance.Our findings not only offer practical guidance for the design of high-efficiency catalysts but also bring a new understanding of the exceptional performance of WGS in a holistic view,which shows a great application potential in materials and catalysis.展开更多
Interfacial ferroelectricity is a recently established mechanism for generating spontaneous reversible electric polarization,arising from the charge transfer between stacked van der Waals layered atomic crystals.It ha...Interfacial ferroelectricity is a recently established mechanism for generating spontaneous reversible electric polarization,arising from the charge transfer between stacked van der Waals layered atomic crystals.It has been realized in both naturally formed multilayer crystals and moirésuperlattices.Owing to the large number of material choices and combinations,this approach is highly versatile,greatly expanding the scope of ultrathin ferroelectrics.A key advantage of interfacial ferroelectricity is its potential to couple with preexisting properties of the constituent layers,enabling their electrical manipulation through ferroelectric switching and paving the way for advanced device functionalities.This review article summarizes recent experimental progress in interfacial ferroelectricity,with an emphasis on its coupling with a variety of electronic properties.After introducing the underlying mechanism of interfacial ferroelectricity and the range of material systems discovered to date,we highlight selected examples showcasing ferroelectric control of excitonic optical properties,Berry curvature effects,and superconductivity.We also discuss the challenges and opportunities that await further studies in this field.展开更多
Surface engineering plays a crucial role in improving the performance of high energy materials,and polydopamine(PDA)is widely used in the field of energetic materials for surface modification and functionalization.In ...Surface engineering plays a crucial role in improving the performance of high energy materials,and polydopamine(PDA)is widely used in the field of energetic materials for surface modification and functionalization.In order to obtain high-quality HMX@PDA-based PBX explosives with high sphericity and a narrow particle size distribution,composite microspheres were prepared using co-axial droplet microfluidic technology.The formation mechanism,thermal behavior,mechanical sensitivity,electrostatic spark sensitivity,compressive strength,and combustion performance of the microspheres were investigated.The results show that PDA can effectively enhance the interfacial interaction between the explosive particles and the binder under the synergistic effect of chemical bonds and the physical"mechanical interlocking"structure.Interface reinforcement causes the thermal decomposition temperature of the sample microspheres to move to a higher temperature,with the sensitivity to impact,friction,and electrostatic sparks(for S-1)increasing by 12.5%,31.3%,and 81.5%respectively,and the compressive strength also increased by 30.7%,effectively enhancing the safety performance of the microspheres.Therefore,this study provides an effective and universal strategy for preparing high-quality functional explosives,and also provides some reference for the safe use of energetic materials in practical applications.展开更多
The unique structure and formation mechanism of medium-entropy alloys(MEAs)generally result in bet-ter comprehensive properties than traditional alloys.However,the strength-ductility trade-offremains a bottleneck,whic...The unique structure and formation mechanism of medium-entropy alloys(MEAs)generally result in bet-ter comprehensive properties than traditional alloys.However,the strength-ductility trade-offremains a bottleneck,which limits their applications.In this study,we designed novel high-performance CrNiCu x MEAs with a heterophase composition by incorporating a Cu-rich phase,and they were fabricated using laser-directed energy deposition(LDED).The results show that synergistic strengthening from multiple phases significantly improved the mechanical properties of the alloys,resulting in a tensile strength of 675 MPa and a ductility of 34.4%,demonstrating an excellent combination of high tensile strength and ductility.The improved mechanical properties of the CrNiCu x medium-entropy alloys are primarily due to the heterophase interfacial strengthening mechanism.In the alloy,numerous semi-coherent and coher-ent interfaces formed between the Cr-rich phase,Cu-rich phase,and the matrix,creating extensive lattice distortions at the interfaces.An increase in the Cu-rich phase content promoted the interaction between phases,enhancing the strain energy of the alloy and the barrier strength of the interfaces.The calcu-latedτint values,ranging from approximately 5.92-6.69 GPa,are significantly higher than those found in traditional alloys,providing a benchmark for designing new high-performance medium-entropy alloys.展开更多
Recently,hollow carbon nanospheres(HCSs)have garnered significant attention as potential Li metal hosts owing to their unique large voids and ease of fabrication.However,similar to other nanoscale hosts,their practica...Recently,hollow carbon nanospheres(HCSs)have garnered significant attention as potential Li metal hosts owing to their unique large voids and ease of fabrication.However,similar to other nanoscale hosts,their practical performance is limited by inhomogeneous agglomeration,increased binder requirements,and high tortuosity within the electrode.To overcome these problems and high tortuosity within the electrode,this study introduces a pomegranate-like carbon microcluster composed of primary HCSs(P-CMs)as a novel Li metal host.This unique nanostructure can be easily prepared using the spray-drying technique,enabling its mass production.Comprehensive analyses with various tools demonstrate that compared with HCS hosts,the P-CM host requires a smaller amount of binder to fabricate a sufficiently robust and even surface electrode.Furthermore,owing to reduced tortuosity,the well-designed P-CM electrode can provide continuous and shortened pathways for electron/ion transport,accelerating the Li-ion transfer kinetics and prohibiting preferential Li plating at the upper region of the electrode.Due to these characteristics,Li metal can be effectively encapsulated in the large inner voids of the primary HCSs constituting the P-CM,thereby enhancing the electrochemical performance of P-CM hosts in Li metal batteries.Specifically,the Coulombic efficiency of the P-CM host can be maintained at 97%over 100 cycles,with a high Li deposition areal capacity of 3 mAh·cm^(-2)and long cycle life(1000 h,1 mA·cm^(-2),and 1.0 mAh·cm^(-2)).Furthermore,a full cell incorporating a LiFePO4 cathode exhibits excellent cycle life.展开更多
Through strategies such as process optimization,solvent selection,and component tuning,the crystallization of perovskite materials has been effectively controlled,enabling perovskite solar cells(PSCs)to achieve over 2...Through strategies such as process optimization,solvent selection,and component tuning,the crystallization of perovskite materials has been effectively controlled,enabling perovskite solar cells(PSCs)to achieve over 25%power conversion efficiency(PCE).However,as PCE continues to improve,interfacial issues within the devices have emerged as critical bottlenecks,hindering further performance enhancements.Recently,interfacial engineering has driven transformative progress,pushing PCEs to nearly 27%.Building upon these developments,this review first summarizes the pivotal role of interfacial modifications in elevating device performance and then,as a starting point,provides a comprehensive overview of recent advancements in normal,inverted,and tandem structure devices.Finally,based on the current progress of PSCs,preliminary perspectives on future directions are presented.展开更多
Four glycoluril-based amphiphilic molecular clips(AMCs)M1~M4 have been prepared for intracellular delivery of short DNA.M1~M4 have two methyl groups on its convex surface and four cations on its aromatic side arm,whic...Four glycoluril-based amphiphilic molecular clips(AMCs)M1~M4 have been prepared for intracellular delivery of short DNA.M1~M4 have two methyl groups on its convex surface and four cations on its aromatic side arm,which can be used to construct self-assembled nanoparticles in aqueous solution driven by hydrophobic interaction.Dynamic light scattering experiments show that M1 and M2 can be driven hydrophobically to aggregate into extremely stable nanoparticles in water at the micromolar concentrations.Fluorescence titration and zeta potential experiments support that the nanoparticles formed by M1 and M2 are able to efficiently encapsulate short DNA(sDNA).Fluorescence imaging and flow cytometry studies reveal that their nano sizes enable intracellular delivery of the encapsulated sDNA into both normal and cancer cells,with delivery percentage reaching up to 94%,while in vitro experiments indicate that the two compounds have excellent biocompatibility and low cytotoxicity.展开更多
The highly selective catalytic hydrogenation of halogenated nitroaromatics was achieved by employing Pd‑based catalysts that were co‑modified with organic and inorganic ligands.It was demonstrated that the catalysts c...The highly selective catalytic hydrogenation of halogenated nitroaromatics was achieved by employing Pd‑based catalysts that were co‑modified with organic and inorganic ligands.It was demonstrated that the catalysts contained Pd species in mixed valence states,with high valence Pd at the metal‑support interface and zero valence Pd at the metal surface.While the strong coordination of triphenylphosphine(PPh3)to Pd0 on the Pd surface prevents the adsorption of halogenated nitroaromatics and thus dehalogenation,the coordination of sodium metavanadate(NaVO3)to high‑valence Pd sites at the interface helps to activate H2 in a heterolytic pathway for the selective hydrogenation of nitro‑groups.The excellent catalytic performance of the interfacial active sites enables the selective hydrogenation of a wide range of halogenated nitroaromatics.展开更多
Large-area two-dimensional(2D)materials,such as graphene,MoS_(2),WS_(2),h-BN,black phosphorus,and MXenes,are a class of advanced materials with many possible applications.Different applications need different substrat...Large-area two-dimensional(2D)materials,such as graphene,MoS_(2),WS_(2),h-BN,black phosphorus,and MXenes,are a class of advanced materials with many possible applications.Different applications need different substrates,and each substrate may need a different way of transferring the 2D material onto it.Problems such as local stress concentrations,an uneven surface tension,inconsistent adhesion,mechanical damage and contamination during the transfer can adversely affect the quality and properties of the transferred material.Therefore,how to improve the integrity,flatness and cleanness of large area 2D materials is a challenge.In order to achieve high-quality transfer,the main concern is to control the interface adhesion between the substrate,the 2D material and the transfer medium.This review focuses on this topic,and finally,in order to promote the industrial use of large area 2D materials,provides a recipe for this transfer process based on the requirements of the application,and points out the current problems and directions for future development.展开更多
Achieving industrial-level electrochemical CO_(2)reduction to formate remains a significant challenge due to limitations in catalyst selectivity and interfacial proton management at high current densities.In a recent ...Achieving industrial-level electrochemical CO_(2)reduction to formate remains a significant challenge due to limitations in catalyst selectivity and interfacial proton management at high current densities.In a recent study,Prof.Guo and colleagues report the development of Turingstructured electrocatalysts,which incorporate reaction-diffusion-inspired topologies to engineer mesoscale surface patterns.This design enables precise modulation of the interfacial microenvironment,enhancing CO_(2)activation and suppressing competing hydrogen evolution.The resulting catalysts achieve efficient and stable CO_(2)-to-formate conversion under industrially relevant conditions,offering a promising strategy for scalable carbon-neutral chemical production.展开更多
Nowadays,high-stable and ultrasensitive heavy metal detection is of utmost importance in water quality monitoring.Nanoparticle-enhanced laser-induced breakdown spectroscopy(NELIBS)shows high potential in hazardous met...Nowadays,high-stable and ultrasensitive heavy metal detection is of utmost importance in water quality monitoring.Nanoparticle-enhanced laser-induced breakdown spectroscopy(NELIBS)shows high potential in hazardous metal detection,however,encounters unstable and weak signals due to nonuniform distribution of analytes.Herein,we developed an interface self-assembly(ISA)method to create a uniformly distributed gold nanolayer at a liquid-liquid interface for positive heavy metal ions capture and NELIBS analysis.The electrostatically selfassembled Au nanoparticles(NPs)-analytes membrane was prepared at the oil-water interface by injecting ethanol into the mixture of cyclohexane and Au NPs-analytes water solution.Then,the interface self-assembled Au NPs-analytes membrane was transformed onto a laser-processed superhydrophilic Si slide for detection.Three heavy metals(cadmium(Cd),barium(Ba),and chromium(Cr))were analyzed to evaluate the stability and sensitivity of the ISA method for NELIBS.The results(Cd:RSD=3.6%,LoD=0.654 mg/L;Ba:RSD=3.4%,LoD=0.236 mg/L;Cr:RSD=7.7%,LoD=1.367 mg/L)demonstrated signal enhancement and high-stable and ultrasensitive detection.The actual sample detection(Cd:RE=7.71%,Ba:RE=6.78%)illustrated great reliability.The ISA method,creating a uniform distribution of NP-analytes at the interface,has promising prospects in NELIBS.展开更多
Recent advances in van der Waals(vdW) ferroelectrics have sparked the development of related heterostructures with non-volatile and field-tunable functionalities. In vdW ferroelectric heterojunctions, the interfacial ...Recent advances in van der Waals(vdW) ferroelectrics have sparked the development of related heterostructures with non-volatile and field-tunable functionalities. In vdW ferroelectric heterojunctions, the interfacial electrical characteristics play a crucial role in determining their performance and functionality. In this study,we explore the interfacial polarization coupling in two-dimensional(2D) ferroelectric heterojunctions by fabricating a graphene/h-BN/CuInP_(2)S_(6)/α-In_(2)Se_(3)/Au ferroelectric field-effect transistor. By varying the gate electric field, the CuInP_(2)S_(6)/α-In_(2)Se_(3) heterojunction displays distinct interfacial polarization coupling states, resulting in significantly different electrical transport behaviors. Under strong gate electric fields, the migration of Cu ions further enhances the interfacial polarization effect, enabling continuous tuning of both the polarization state and carrier concentration in α-In_(2)Se_(3). Our findings offer valuable insights for the development of novel multifunctional devices based on 2D ferroelectric materials.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22272118,22172111,and 22309134)the Science and Technology Commission of Shanghai Municipality,China(Nos.22ZR1464100,20ZR1460300,and 19DZ2271500)+2 种基金the China Postdoctoral Science Foundation(2022M712402),the Shanghai Rising-Star Program(23YF1449200)the Zhejiang Provincial Science and Technology Project(2022C01182)the Fundamental Research Funds for the Central Universities(2023-3-YB-07)。
文摘Carbon superstructures with multiscale hierarchies and functional attributes represent an appealing cathode candidate for zinc hybrid capacitors,but their tailor-made design to optimize the capacitive activity remains a confusing topic.Here we develop a hydrogen-bond-oriented interfacial super-assembly strategy to custom-tailor nanosheet-intertwined spherical carbon superstructures(SCSs)for Zn-ion storage with double-high capacitive activity and durability.Tetrachlorobenzoquinone(H-bond acceptor)and dimethylbenzidine(H-bond donator)can interact to form organic nanosheet modules,which are sequentially assembled,orientally compacted and densified into well-orchestrated superstructures through multiple H-bonds(N-H···O).Featured with rich surface-active heterodiatomic motifs,more exposed nanoporous channels,and successive charge migration paths,SCSs cathode promises high accessibility of built-in zincophilic sites and rapid ion diffusion with low energy barriers(3.3Ωs-0.5).Consequently,the assembled Zn||SCSs capacitor harvests all-round improvement in Zn-ion storage metrics,including high energy density(166 Wh kg-1),high-rate performance(172 m Ah g^(-1)at 20 A g^(-1)),and long-lasting cycling lifespan(95.5%capacity retention after 500,000 cycles).An opposite chargecarrier storage mechanism is rationalized for SCSs cathode to maximize spatial capacitive charge storage,involving high-kinetics physical Zn^(2+)/CF_(3)SO_(3)-adsorption and chemical Zn^(2+)redox with carbonyl/pyridine groups.This work gives insights into H-bond-guided interfacial superassembly design of superstructural carbons toward advanced energy storage.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.22173051,21829301,21774066)College Discipline Innovation and Intelligence Introduction Program(111 Project(B16027)+1 种基金the International Cooperation Base(2016D01025)Tianjin International Joint Research and Development Center。
文摘Spatial confinement of block copolymers can induce frustrations,which can further be utilized to regulate self-assembled structures,thus providing an efficient route for fabricating novel structures.We studied the self-assembly of AB di-block copolymers(di-BCPs)confined in Janus spherical nanocavities using simulations,and explained the structure formation mechanisms.In the case of a strongly selective cavity wall,all the lamella-forming,gyroid-forming,and cylinder-forming di-BCPs can form interfacial frustration-induced Janus concentric perforated lamellar nanoparticles,whose outermost is a Janus spherical shell and the internal is a sphere with concentric perforated lamellar structure.In particular,Janus concentric perforated lamellar nanoparticles with holes distributed only near the equatorial plane were obtained in both lamella-forming and gyroid-forming di-BCPs,directly reflecting the effect of interfacial frustration.The minority-block domain of the cylider-forming di-BCPs may form hemispherical perforated lamellar structures with holes distributed in parallel layers with a specific orientation.For symmetric di-BCPs,both the A and B domains in each nanoparticle are continuous,interchangeable,and have rotational symmetry.While for gyroid-forming and cylinder-forming di-BCPs,only the majority-block domains are continuous in each nanoparticle,and holes in the minority-block domains usually have rotational symmetry.In the case of a weakly selective cavity wall,the inhomogeneity of the cavity wall results in structures having a specific orientation(such as flower-like and branched structures in gyroid-forming and cylinder-forming di-BCPs)and a perforated wetting layer with uniformly distributed holes.The novel nanoparticles obtained may have potential applications in nanotechnology as functional nanostructures or nanoparticles.
基金Y.Zhan acknowledges funding support from the National Key Research and Development Program of China(2022YFE0137400)the National Natural Science Foundation of China(62274040)+5 种基金A.Yu acknowledges funding support from the National Natural Science Foundation of China(62304046)the National Key Research and Development Program of China(2022YFB2802802)the Key Laboratory of Rare Earths,Ganjiang Innovation Academy,Chinese Academy of SciencesX.Zhang acknowledges funding from the China Postdoctoral Science Foundation(GZC20230463)X.Li acknowledges funding from the China Postdoctoral Science Foundation(GZC20230461)We also acknowledge support from the Shanghai Science and Technology Innovation Action Plan 2023 Special Project for Supporting Carbon Peak Carbon Neutrality Project(23DZ1200400).
文摘The NiOx,due to its excellent semiconductor properties,ease of large-area deposition,and tunable optoelectronic characteristics,shows great potential in industrial large-area perovskite technologies.However,NiO_(x)-based perovskite solar cells(PSCs)are limited by interfacial photocatalytic chemical reactions and energy level mismatch.Thus,phosphate-based self-assembled monolayers(SAMs)have been widely developed for delicate interfacial modification;however,they suffer from severe issues such as self-aggregation and high cost.Herein,a low-cost carboxylate-based SAM(pyrenebutyric acid,PyBA)was used to modify NiO_(x),achieving an improved surface chemical environment and interfacial properties,such as an increased Ni^(3+)/Ni2^(+)ratio,a reduced proportion of high-valence Ni^(≥3+),and better-aligned hole transport interface energy level.The introduction of PyBA also results in larger grain size,higher uniformity,and enhanced photoluminescence(PL)from the bottom of the perovskite,yielding a significant increase in efficiency from an initial 22.48%to 25.14%,while increasing the open-circuit voltage(VOC)from 1.077 to 1.192 V.Additionally,a perovskite module with an aperture area of 21 cm^(2)achieved an efficiency of 22.28%,demonstrating the excellent scalability of the PyBA treatment.Moreover,the well-modified buried interface combined with the chemical inertness and structural rigidity of pyrene ensures excellent ultraviolet(UV)stability(the target module maintained 92%of the initial efficiency after 200 h and the control device only retained 40%).
基金This work was financially supported by the National Nat-ural Science Foundation of China(Grant Nos.52072193 and U22A20131)the Shandong Provincial Natural Science Foundation(Grant Nos.ZR2021JQ16 and ZR2019YQ19)+2 种基金the Project of Shan-dong Province Higher Educational Science and Technology Program(Grant No.2019KJA026)the State Key Laboratory for Modification of Chemical Fibers and Polymer Materials(Grant No.KF2217)the Science Fund of Shandong Laboratory of Yantai Advanced Materials and Green Manufacturing(Grant No.AMGM2021F11).
文摘The interfacial property of carbon fiber(CF)reinforced composites is crucial to facilitate the application of high-strength composites.Utilizing the electrostatic and hydrogen bond properties of diazo resin,carbon nanotubes(CNTs)and graphene oxide(GO)could be quickly grafted onto the surface of the CF via the layer-by-layer self-assembly technique.The results showed that CNTs and GO were uniformly coated onto the CF surface,and the chemical activity and roughness of the modified CF surface were improved signif-icantly.The modified CF surface can significantly augment the interaction between the epoxy resin and the fiber.Remarkably,due to the good interfacial property,the impact performance of the composites re-inforced with the nanomaterial-modified CF was improved obviously.In addition,the interface properties of the composites are studied in depth.This method is expected to achieve rapid surface modification of carbon fiber.
基金support from the National Natural Science Foundation of China(21890734,21890730 and 21971247)Youth Innovation Promotion Association CAS(2019036)
文摘The chiral self-assembly of functional molecules,polymers and clus-ters into nanoscale objects with well-defined ordering,asymmetry and in some cases out-of-equilibrium characteristics is an important strategy to fabricate novel materials[1],which might address key challenges at the heart of energy,environmental and biomedical applications.In recent years,subsequent utilization of these nanoscale units as new building blocks to fabricate advanced structures and realize more complex func-tions like those in the biology systems has aroused interests.These at-tempts are originated from the concept of molecular nanotechnology but have gone beyond its boundaries towards the breakthroughs of self-assembled machines,advanced nanoarchitectonics and molecular nanotopology[2,3].
基金supported by the National Natural Science Foundation of China(Nos.52122315,21972008)Beijing Nova Program(No.Z201100006820021).
文摘Wettability transition is a significant responsive mechanism which is widely applied to construct smart materials and systems.The broad-spectrum responsiveness of the wettability transition makes it a promising way to expand innovative applications.Here,we develop a track-guided self-transportation system mediated by sequential wettability transition accompanied with capillary transportation.Alkaline fuel is loaded into polydimethylsiloxane(PDMS)cuboid to trigger the wettability transition of distributed superhydrophobic tracks laid in shallow water.After the wettability transition,the induced capillary force can propel the repetitive track-to-track transportation of PDMS.Importantly,the spacing between adjacent tracks is rationally designed based on multiple factors including threshold of wettability transition,diffusion kinetics and capillary interaction.Furthermore,the track-guided transportation system is applied to realize directed self-assembly of multiple PDMS building blocks for designated configuration,which increases the complexity and intelligence of self-assembly systems.
基金supported by Zhejiang Provincial Natural Science Foundation of China(No.LR23C160001)Scientific Research Startup Foundation of Zhejiang Ocean University(No.11034150220006).
文摘The utilization of solar-driven interfacial evaporation technology is highly important in addressing the energy crisis and water scarcity,primarily because of its affordability and minimal energy usage.Enhancing the performance of solar energy evaporation and minimizing material degradation during application can be achieved through the design of novel photothermal materials.In solar interfacial evaporation,photothermal materials exhibit a wide range of additional characteristics,but a systematic overview is lacking.This paper encompasses an examination of various categories and principles pertaining to photothermal materials,as well as the structural design considerations for salt-resistant materials.Additionally,we discuss the versatile uses of this appealing technology in different sectors related to energy and the environment.Furthermore,potential solutions to enhance the durability of photothermal materials are also highlighted,such as the rational design of micro/nano-structures,the use of adhesives,the addition of anti-corrosion coatings,and the preparation of self-healing surfaces.The objective of this review is to offer a viable resolution for the logical creation of high-performance photothermal substances,presenting a guide for the forthcoming advancement of solar evaporation technology.
文摘NiO_(x)as a hole transport material for inverted perovskite solar cells has received great attention owing to its high transparency,low fabrication temperature,and superior stability.However,the mismatched energy levels and possible redox reactions at the NiO_(x)/perovskite interface severely limit the performance of NiO_(x) based inverted perovskite solar cells.Herein,we introduce a p-type self-assembled monolayer between NiO_(x)and perovskite layers to modify the interface and block the undesirable redox reaction between perovskite and NiO_(x)The selfassembled monolayer molecules all contain phosphoric acid function groups,which can be anchored onto the NiOr surface and passivate the surface defect.Moreover,the introduction of self-assembled monolayers can regulate the energy level structure of NiO_(x),reduce the interfacial band energy offset,and hence promote the hole transport from perovskite to NiO_(x)layer.Consequently,the device performance is significantly enhanced in terms of both power conversion efficiency and stability.
文摘Revealing the structure evolution of interfacial active species during a dynamic catalytic process is a challenging but pivotal issue for the rational design of high-performance catalysts.Here,we successfully prepare sub-nanometric Pt clusters(~0.8 nm)encapsulated within the defects of CeO_(2)nanorods via an in-situ defect engineering methodology.The as-prepared Pt@d-CeO_(2)catalyst significantly boosts the activity and stability in the water-gas shift(WGS)reaction compared to other analogs.Based on controlled experiments and complementary(in-situ)spectroscopic studies,a reversible encapsulation induced by active site transformation between the Pt^(2+)-terminal hydroxyl and Pt^(δ+)-O vacancy species at the interface is revealed,which enables to evoke the enhanced performance.Our findings not only offer practical guidance for the design of high-efficiency catalysts but also bring a new understanding of the exceptional performance of WGS in a holistic view,which shows a great application potential in materials and catalysis.
基金Project supported by the Natural Science Foundation of Jiangsu Province(Grant Nos.BK20231529 and BK20233001)the National Key Research and Development Program of China(Grant No.2024YFA1409100)+2 种基金the Fundamental Research Funds for the Central Universities(Grant No.0204-14380233)the National Natural Science Foundation of China(Grant Nos.12474170 and 123B2059)the National Postdoctoral Program for Innovative Talents(Grant No.BX20240160)。
文摘Interfacial ferroelectricity is a recently established mechanism for generating spontaneous reversible electric polarization,arising from the charge transfer between stacked van der Waals layered atomic crystals.It has been realized in both naturally formed multilayer crystals and moirésuperlattices.Owing to the large number of material choices and combinations,this approach is highly versatile,greatly expanding the scope of ultrathin ferroelectrics.A key advantage of interfacial ferroelectricity is its potential to couple with preexisting properties of the constituent layers,enabling their electrical manipulation through ferroelectric switching and paving the way for advanced device functionalities.This review article summarizes recent experimental progress in interfacial ferroelectricity,with an emphasis on its coupling with a variety of electronic properties.After introducing the underlying mechanism of interfacial ferroelectricity and the range of material systems discovered to date,we highlight selected examples showcasing ferroelectric control of excitonic optical properties,Berry curvature effects,and superconductivity.We also discuss the challenges and opportunities that await further studies in this field.
基金supported by the National Natural Science Foundation of China(Grant No.22005275).
文摘Surface engineering plays a crucial role in improving the performance of high energy materials,and polydopamine(PDA)is widely used in the field of energetic materials for surface modification and functionalization.In order to obtain high-quality HMX@PDA-based PBX explosives with high sphericity and a narrow particle size distribution,composite microspheres were prepared using co-axial droplet microfluidic technology.The formation mechanism,thermal behavior,mechanical sensitivity,electrostatic spark sensitivity,compressive strength,and combustion performance of the microspheres were investigated.The results show that PDA can effectively enhance the interfacial interaction between the explosive particles and the binder under the synergistic effect of chemical bonds and the physical"mechanical interlocking"structure.Interface reinforcement causes the thermal decomposition temperature of the sample microspheres to move to a higher temperature,with the sensitivity to impact,friction,and electrostatic sparks(for S-1)increasing by 12.5%,31.3%,and 81.5%respectively,and the compressive strength also increased by 30.7%,effectively enhancing the safety performance of the microspheres.Therefore,this study provides an effective and universal strategy for preparing high-quality functional explosives,and also provides some reference for the safe use of energetic materials in practical applications.
基金supported by the National Natural Science Foundation of China(Grant No.U2341254)the National Natural Science Foundation of China(Grant No.52071124),the Natural Science Foundation of Jiangsu Province(No.BK20230502)the Jiangsu Funding Program for Excellent Postdoctoral Talent(No.2022ZB547).
文摘The unique structure and formation mechanism of medium-entropy alloys(MEAs)generally result in bet-ter comprehensive properties than traditional alloys.However,the strength-ductility trade-offremains a bottleneck,which limits their applications.In this study,we designed novel high-performance CrNiCu x MEAs with a heterophase composition by incorporating a Cu-rich phase,and they were fabricated using laser-directed energy deposition(LDED).The results show that synergistic strengthening from multiple phases significantly improved the mechanical properties of the alloys,resulting in a tensile strength of 675 MPa and a ductility of 34.4%,demonstrating an excellent combination of high tensile strength and ductility.The improved mechanical properties of the CrNiCu x medium-entropy alloys are primarily due to the heterophase interfacial strengthening mechanism.In the alloy,numerous semi-coherent and coher-ent interfaces formed between the Cr-rich phase,Cu-rich phase,and the matrix,creating extensive lattice distortions at the interfaces.An increase in the Cu-rich phase content promoted the interaction between phases,enhancing the strain energy of the alloy and the barrier strength of the interfaces.The calcu-latedτint values,ranging from approximately 5.92-6.69 GPa,are significantly higher than those found in traditional alloys,providing a benchmark for designing new high-performance medium-entropy alloys.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(No.2020R1C1C1003375)。
文摘Recently,hollow carbon nanospheres(HCSs)have garnered significant attention as potential Li metal hosts owing to their unique large voids and ease of fabrication.However,similar to other nanoscale hosts,their practical performance is limited by inhomogeneous agglomeration,increased binder requirements,and high tortuosity within the electrode.To overcome these problems and high tortuosity within the electrode,this study introduces a pomegranate-like carbon microcluster composed of primary HCSs(P-CMs)as a novel Li metal host.This unique nanostructure can be easily prepared using the spray-drying technique,enabling its mass production.Comprehensive analyses with various tools demonstrate that compared with HCS hosts,the P-CM host requires a smaller amount of binder to fabricate a sufficiently robust and even surface electrode.Furthermore,owing to reduced tortuosity,the well-designed P-CM electrode can provide continuous and shortened pathways for electron/ion transport,accelerating the Li-ion transfer kinetics and prohibiting preferential Li plating at the upper region of the electrode.Due to these characteristics,Li metal can be effectively encapsulated in the large inner voids of the primary HCSs constituting the P-CM,thereby enhancing the electrochemical performance of P-CM hosts in Li metal batteries.Specifically,the Coulombic efficiency of the P-CM host can be maintained at 97%over 100 cycles,with a high Li deposition areal capacity of 3 mAh·cm^(-2)and long cycle life(1000 h,1 mA·cm^(-2),and 1.0 mAh·cm^(-2)).Furthermore,a full cell incorporating a LiFePO4 cathode exhibits excellent cycle life.
基金supported by National Natural Science Foundation of China(52302229,62404072)the Key Lab of Modern Optical Technologies of Education Ministry of China,Soochow University(KJS2425)+1 种基金Doctoral Foundation of Henan Polytech-nic University(B2024-72)Science and Technology Research Project of Jiangxi Provincial Department of Education(Grant No.GJJ2400702).
文摘Through strategies such as process optimization,solvent selection,and component tuning,the crystallization of perovskite materials has been effectively controlled,enabling perovskite solar cells(PSCs)to achieve over 25%power conversion efficiency(PCE).However,as PCE continues to improve,interfacial issues within the devices have emerged as critical bottlenecks,hindering further performance enhancements.Recently,interfacial engineering has driven transformative progress,pushing PCEs to nearly 27%.Building upon these developments,this review first summarizes the pivotal role of interfacial modifications in elevating device performance and then,as a starting point,provides a comprehensive overview of recent advancements in normal,inverted,and tandem structure devices.Finally,based on the current progress of PSCs,preliminary perspectives on future directions are presented.
文摘Four glycoluril-based amphiphilic molecular clips(AMCs)M1~M4 have been prepared for intracellular delivery of short DNA.M1~M4 have two methyl groups on its convex surface and four cations on its aromatic side arm,which can be used to construct self-assembled nanoparticles in aqueous solution driven by hydrophobic interaction.Dynamic light scattering experiments show that M1 and M2 can be driven hydrophobically to aggregate into extremely stable nanoparticles in water at the micromolar concentrations.Fluorescence titration and zeta potential experiments support that the nanoparticles formed by M1 and M2 are able to efficiently encapsulate short DNA(sDNA).Fluorescence imaging and flow cytometry studies reveal that their nano sizes enable intracellular delivery of the encapsulated sDNA into both normal and cancer cells,with delivery percentage reaching up to 94%,while in vitro experiments indicate that the two compounds have excellent biocompatibility and low cytotoxicity.
文摘The highly selective catalytic hydrogenation of halogenated nitroaromatics was achieved by employing Pd‑based catalysts that were co‑modified with organic and inorganic ligands.It was demonstrated that the catalysts contained Pd species in mixed valence states,with high valence Pd at the metal‑support interface and zero valence Pd at the metal surface.While the strong coordination of triphenylphosphine(PPh3)to Pd0 on the Pd surface prevents the adsorption of halogenated nitroaromatics and thus dehalogenation,the coordination of sodium metavanadate(NaVO3)to high‑valence Pd sites at the interface helps to activate H2 in a heterolytic pathway for the selective hydrogenation of nitro‑groups.The excellent catalytic performance of the interfacial active sites enables the selective hydrogenation of a wide range of halogenated nitroaromatics.
基金the National Key R&D Program of China(2022YFA1505200)the National Natural Science Foundation of China(22472140,22021001)the Fundamental Research Funds for the Central Universities(20720210017 and 20720210009)。
文摘Large-area two-dimensional(2D)materials,such as graphene,MoS_(2),WS_(2),h-BN,black phosphorus,and MXenes,are a class of advanced materials with many possible applications.Different applications need different substrates,and each substrate may need a different way of transferring the 2D material onto it.Problems such as local stress concentrations,an uneven surface tension,inconsistent adhesion,mechanical damage and contamination during the transfer can adversely affect the quality and properties of the transferred material.Therefore,how to improve the integrity,flatness and cleanness of large area 2D materials is a challenge.In order to achieve high-quality transfer,the main concern is to control the interface adhesion between the substrate,the 2D material and the transfer medium.This review focuses on this topic,and finally,in order to promote the industrial use of large area 2D materials,provides a recipe for this transfer process based on the requirements of the application,and points out the current problems and directions for future development.
基金financially supported by the National Natural Science Foundation of China(No.22209024)Tongcheng R&D Foundation(No.CPCIF-RA-0102)the State Key Laboratory of Advanced Fiber Materials,Donghua University
文摘Achieving industrial-level electrochemical CO_(2)reduction to formate remains a significant challenge due to limitations in catalyst selectivity and interfacial proton management at high current densities.In a recent study,Prof.Guo and colleagues report the development of Turingstructured electrocatalysts,which incorporate reaction-diffusion-inspired topologies to engineer mesoscale surface patterns.This design enables precise modulation of the interfacial microenvironment,enhancing CO_(2)activation and suppressing competing hydrogen evolution.The resulting catalysts achieve efficient and stable CO_(2)-to-formate conversion under industrially relevant conditions,offering a promising strategy for scalable carbon-neutral chemical production.
基金supported by the National Natural Science Foundation of China(No.62075069 and 52303092)the Water Conservancy Technology project of Hunan Province,China(XSKJ2021000-32)+1 种基金the City University of Hong Kong(#7005507)the Open Project of Yunnan Precious Metals Laboratory Co.,Ltd(grant number YPML-2023050278).
文摘Nowadays,high-stable and ultrasensitive heavy metal detection is of utmost importance in water quality monitoring.Nanoparticle-enhanced laser-induced breakdown spectroscopy(NELIBS)shows high potential in hazardous metal detection,however,encounters unstable and weak signals due to nonuniform distribution of analytes.Herein,we developed an interface self-assembly(ISA)method to create a uniformly distributed gold nanolayer at a liquid-liquid interface for positive heavy metal ions capture and NELIBS analysis.The electrostatically selfassembled Au nanoparticles(NPs)-analytes membrane was prepared at the oil-water interface by injecting ethanol into the mixture of cyclohexane and Au NPs-analytes water solution.Then,the interface self-assembled Au NPs-analytes membrane was transformed onto a laser-processed superhydrophilic Si slide for detection.Three heavy metals(cadmium(Cd),barium(Ba),and chromium(Cr))were analyzed to evaluate the stability and sensitivity of the ISA method for NELIBS.The results(Cd:RSD=3.6%,LoD=0.654 mg/L;Ba:RSD=3.4%,LoD=0.236 mg/L;Cr:RSD=7.7%,LoD=1.367 mg/L)demonstrated signal enhancement and high-stable and ultrasensitive detection.The actual sample detection(Cd:RE=7.71%,Ba:RE=6.78%)illustrated great reliability.The ISA method,creating a uniform distribution of NP-analytes at the interface,has promising prospects in NELIBS.
基金supported by the Chinese Academy of Sciences Project for Young Scientists in Basic Research(Grant No.YSBR-049)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302800)the Fundamental Research Funds for the Central Universities(Grant No.WK3510000013)。
文摘Recent advances in van der Waals(vdW) ferroelectrics have sparked the development of related heterostructures with non-volatile and field-tunable functionalities. In vdW ferroelectric heterojunctions, the interfacial electrical characteristics play a crucial role in determining their performance and functionality. In this study,we explore the interfacial polarization coupling in two-dimensional(2D) ferroelectric heterojunctions by fabricating a graphene/h-BN/CuInP_(2)S_(6)/α-In_(2)Se_(3)/Au ferroelectric field-effect transistor. By varying the gate electric field, the CuInP_(2)S_(6)/α-In_(2)Se_(3) heterojunction displays distinct interfacial polarization coupling states, resulting in significantly different electrical transport behaviors. Under strong gate electric fields, the migration of Cu ions further enhances the interfacial polarization effect, enabling continuous tuning of both the polarization state and carrier concentration in α-In_(2)Se_(3). Our findings offer valuable insights for the development of novel multifunctional devices based on 2D ferroelectric materials.
