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
Peptide-based assemblies have gained increasing attention in different areas of nanotechnology,drug delivery and molecular biology.Among these,non-natural β-peptide scaffolds are particularly promising,as their progr...Peptide-based assemblies have gained increasing attention in different areas of nanotechnology,drug delivery and molecular biology.Among these,non-natural β-peptide scaffolds are particularly promising,as their programmable and diverse secondary structures,high metabolic stability and strong self-association propensity can be easily exploited to create variable constructs.We have recently demonstrated that heterochiral,acyclic β^(3)-peptides assembled into striped lamellar nanostructures that induced antibacterial activity.The process of this assembly formation could be exploited in diverse areas,however identifying oligomerisation stages,and more importantly,controlling the spontaneous process at different levels is still lacking.In this study,a set of analogues heterochiral hexameric β^(3)-peptide sequences was investigated to understand how systematic,small variations of the sequences,such as single point mutation or N-terminal chemical modification,can influence the resulting assemblies and allow the control of formed morphologies.TEM and cryo-EM combined with molecular dynamics simulation enabled the identification and differentiation of morphological stages throughout the entire multi-step process.Depending on the position of the sequence modifications,the self-assembled structures formed small oligomers,individual protofibrils,extended,flat lamellae,bundles and macroscopic clusters.These results outline how the self-assembly process of short heterochiral β-peptides can be qualitatively fine-tuned by sequence modifications,which contribute to understanding the general peptide assembly processes for their fibrillar morphologies.展开更多
The increasing scarcity of freshwater resources has driven the rapid emergence of solar-driven interfacial evaporators(SDIEs)as a sustainable approach to harvest fresh water by utilizing solar energy.Lignocellulosic b...The increasing scarcity of freshwater resources has driven the rapid emergence of solar-driven interfacial evaporators(SDIEs)as a sustainable approach to harvest fresh water by utilizing solar energy.Lignocellulosic biomass,featuring natural abundance,excellent renewability,unique natural structures,and superior biodegradability compared to the synthetic polymers,is highly attractive for constructing solar steam generators.This review aims to offer an innovative and in-depth insight into designing and optimizing highperformance integrated solar interfacial evaporators derived from renewable lignocellulosic biomass.First,the structural characteristics of lignocellulosic biomass are briefly introduced,serving as photothermal layer or supporting substrates in SDIEs.Secondly,the fabrication methods and processing technologies of lignocellulosic biomass-based evaporators are summarized from the perspective of photothermal layer and supporting substrates.Next,the most recent advances of regulation and optimization strategies are proposed to improve evaporation efficiency.Subsequently,this review summarizes the diverse functionalities of SDIEs,including desalination,power generation,wastewater treatment and antimicrobial,atmospheric water harvesting,and photocatalytic hydrogen production.Finally,the challenges in this field and outlook on the future development are discussed,which are anticipated to provide new opportunities for the advancement of lignocellulosic biomass-based SDIEs.展开更多
Sustainability and scalability remain critical hurdles for the commercialization of organic solar cells(OSCs).However,addressing both poses challenge.Herein,we introduce a simple yet effective strategy utilizing 3,5-d...Sustainability and scalability remain critical hurdles for the commercialization of organic solar cells(OSCs).However,addressing both poses challenge.Herein,we introduce a simple yet effective strategy utilizing 3,5-dichloropyridine(PDCC)as a solid additive to fine-tune the self-assembly behavior of Y-series non-fullerene acceptors(NFAs)to tackle the upscaling limitations in green-solvent-processed OSCs.PDCC predominantly interacts with Y-series NFAs,facilitating molecular crystallization and thereby driving the self-assembly of Y-series NFAs during film-forming dynamics,leading to more uniform active layers with improved molecular packing and reduced charge recombination.As a result,PDCC-driven self-assembly strategy enables high-performance OSCs with a power conversion efficiency(PCE)of 20.47%.When translated to sustainable fabrication,this strategy significantly boosts the PCE of large-area green-solvent-processed OSC modules(19.3 cm^(2))from 13.87%to 15.79%,ranking it among the best-performing green-solvent-processed large-area OSC modules(>18 cm^(2)).Beyond its impact on PCE enhancement,PDCC serves as a multifunctional additive to improve long-term stability and exhibits strong universality across multiple material systems.This work establishes a promising approach for advancing sustainable and scalable OSCs,paving the way for their commercialization.展开更多
The rapid advancement of flexible electronics technology has placed higher demands on the structural design and performance regulation of elastic materials.Cellulosic elastomers,with their biodegradability,renewabilit...The rapid advancement of flexible electronics technology has placed higher demands on the structural design and performance regulation of elastic materials.Cellulosic elastomers,with their biodegradability,renewability,and tunability,emerge as ideal candidate materials.Entropy-driven self-as sembly promotes the spontaneous formation of ordered structures,serving as a crucial pathway for optimizing cellulose elastomer properties.However,the structure-property relationship between the self-assembled ordered structures of cellulose elastomers and their mechanical and electrical properties remains insufficiently explored.It hinders the expansion of their applications in electronic devices.This paper systematically reviews the structure-property regulation mechanisms of self-assembled cellulosic elastomers from an entropy-driven perspective.It elucidates the application principles and performance optimization strategies for mechanical energy harvesting and self-powered sensing,while also exploring the challenges and prospects for performance enhancement.This work provides a reference for the development of self-assembled cellulosic elastomers in the field of energy devices.展开更多
The preparation and functionalization of polymeric capsules attract intense attention due to their application in various areas.Herein we presented an amphiphilic alternating copolymer(ACP)-based microcapsule which is...The preparation and functionalization of polymeric capsules attract intense attention due to their application in various areas.Herein we presented an amphiphilic alternating copolymer(ACP)-based microcapsule which is both robust and readily-functionalized through interfacial click polymerization.A water-in-oil emulsion was constructed to act as the reaction medium,the hydrophilic 1,3-butadiene diepoxide(BDE)in water phase reacted with the oleophilic 1,4-dibutanedithiol(BDT)in oil phase at the water-oil interface to form the amphiphilic ACP named poly(2,3-dihydroxy butylene-alt-butylene dithioether)(abbreviated as P(DHB-a-BDT)below),which would deposite in situ to form the micro-sized capsules.Significantly,the dried capsules are robust enough to be rehydrated once the water was added and almost restored their original morphologies.Further elucidation showed that the Young's modulus of these capsules exceeded 1 GPa.As long as we know,it is the first time for the mechanical properties of the ACP-based microstructures being investigated.Besides,functionalization could be achieved simultaneously with the formation process.As a proof of concept,positive-charged capsules were successfully obtained through click copolymerization.Stemming from the unique characteristics of amphiphilic ACPs which combined both merits of click chemistry and interfacial reactions,all these features of the current method as well as the resultant capsules may promote the application of the polymeric capsules.展开更多
Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-...Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.展开更多
Low reactivity and appropriate wettability between molten superalloys and ceramic materials are crucial for the production of high-quality superalloy castings.The sessile-drop experiment was employed to systematically...Low reactivity and appropriate wettability between molten superalloys and ceramic materials are crucial for the production of high-quality superalloy castings.The sessile-drop experiment was employed to systematically investigate the interfacial reaction and wettability between the 4777DS1 superalloy and SiO_(2)-based ceramic core at various temperatures(1,480℃,1,500℃,1,520℃,and 1,550℃).The wetting behavior and interfacial reaction products at different temperatures were analyzed by scanning electron microscopy(SEM),energy dispersive spectroscopy(EDS),and X-ray diffraction(XRD).The interfacial reaction process and products were discussed,and the thermodynamic behavior and interfacial reaction mechanisms were elucidated.The results demonstrate that the wetting behavior and interfacial reaction between the 4777DS1 alloy and the ceramic core are significantly influenced by temperature.The wettability angle exhibits a trend of initial decrease followed by an increase with rising temperature,reaching a maximum of 139°at 1,480℃,indicating poorer wettability of the 4777DS1 superalloy with the ceramic core and better casting properties at this specific temperature.The most intense interfacial reaction occurs at 1,520℃,resulting in the formation of the main interfacial reaction products such as Al_(2)O_(3),SiO_(2),and HfO_(2).Additionally,some crystal-like products rich in Si and Hf distribute on the reaction layer.展开更多
Understanding the intricate interplay between electrode reactivity and interfacial chemistry is crucial for advancing halide perovskite memristors toward practical applications.Here,we systematically investigate how t...Understanding the intricate interplay between electrode reactivity and interfacial chemistry is crucial for advancing halide perovskite memristors toward practical applications.Here,we systematically investigate how top electrode materials(Au,Ag,Cu,Al)influence the resistive switching behavior of quasi-2D CsPbBr_(3) devices through controlled interfacial engineering.By introducing a novel bilayer electrode architecture,we successfully decouple electrode surface oxidation effects from perovskite/electrode interfacial oxidation reactions for the first time.In situ XRD,photoluminescence spectroscopy,and interfacial XPS analysis reveal that voltage-driven bromide ion migration coupled with electrode-dependent reactions governs the switching mechanisms.Chemically inert Au electrodes show no switching due to insufficient interfacial reactivity,while highly reactive Al electrodes cause irreversible degradation through excessive chemical interactions.In contrast,moderately active Ag and Cu electrodes enable stable bipolar switching with dual negative differential resistance characteristics.The optimal performance emerges from balanced electrode reactivity that facilitates reversible interfacial redox reactions without structural degradation.These findings establish fundamental design principles linking electrode chemical activity to device functionality,providing a rational framework for engineering robust perovskite memristors with enhanced stability and performance for next-generation memory and neuromorphic computing applications.展开更多
To develop specific lining materials for rare earth steel nozzles,LaAlO_(3)powder was first synthesized by high-temperature solid-phase synthesis at 1400℃for 3 h using La_(2)O_(3)and Al_(2)O_(3)powders as raw materia...To develop specific lining materials for rare earth steel nozzles,LaAlO_(3)powder was first synthesized by high-temperature solid-phase synthesis at 1400℃for 3 h using La_(2)O_(3)and Al_(2)O_(3)powders as raw materials.Then BN,AlN,Si_(3)N_(4)and TiN powders were pressed intoφ30 mm×7 mm substrate samples under 120 MPa with PVA as the binder.Equal amounts of La_(2)O_(3)and LaAlO_(3)powders were placed on their surfaces,reacting at 1550℃for 3 h in different atmospheres(reducing and argon conditions).The interfacial reactions of the four nitride(BN,Si_(3)N_(4),AlN,and TiN)substrate samples with La_(2)O_(3)and LaAlO_(3)in different atmospheres were studied,respectively.The results show that in reducing and argon atmospheres,the intensity order of the reactions between the four nitrides and La_(2)O_(3)is Si_(3)N_(4)>BN>AlN>TiN.In the reducing atmosphere,the reaction intensity order of the four nitrides with LaAlO_(3)is Si_(3)N_(4)>AlN≈TiN>BN.However,in the argon atmosphere,the order is Si_(3)N_(4)>BN>AlN≈TiN.TiN has good structural stability in both reducing and argon atmospheres,and shows weak reactivity with La_(2)O_(3)and LaAlO_(3).It is a relatively good anti-clogging lining material for rare earth steel nozzles.展开更多
Peroxymonosulfate(PMS)-based advanced oxidation processes(AOPs)are an effective way to remove emerging contaminants(ECs)from water.The catalytic process involving PMS is hindered by the suboptimal electron trans-fer e...Peroxymonosulfate(PMS)-based advanced oxidation processes(AOPs)are an effective way to remove emerging contaminants(ECs)from water.The catalytic process involving PMS is hindered by the suboptimal electron trans-fer efficiency of current catalysts,the further application of AOPs technology is limited.Here,it is proposed that the interfacial electric field can be controlled by bor(B)-doped FeNC catalysts,which shows significant advantages in the efficient generation,release and participation of reactive oxygen species(ROS)in the reaction.The super exchange interaction between Fe sites and N and B sites is realized through the directional transfer of electrons in the interfacial electric field,which ensures the high efficiency and stability of the PMS catalytic process.B doping increases the d orbitals distribution at Fermi level,which facilitates enhanced electron transition activity,thereby promoting the effective generation of (1)^O_(2).At the same time,orbital hybridization causes the center of the d band to move to a lower energy level,which not only contributes to the desorption process of (1)^O_(2),but also accelerates its release.In addition,B-doping also improved the adsorption capacity of organic pollutants and shortened the migration distance of ROS,thereby significantly improving the degradation efficiency of ECs.The B-doping strategy outlined offers a novel approach to the development of FeNC catalysts,it lays a theoretical foundation and offers technical insights for the integration of PMS/AOPs technology in the ECs management.展开更多
Aqueous zinc-ion batteries(AZIBs)offer a safe,cost-effective,and high-capacity energy storage solution,yet their performance is hindered by interfacial challenges at the Zn anode,including hydrogen evolution,corrosion...Aqueous zinc-ion batteries(AZIBs)offer a safe,cost-effective,and high-capacity energy storage solution,yet their performance is hindered by interfacial challenges at the Zn anode,including hydrogen evolution,corrosion,and dendritic Zn growth.While most studies focus on regulating Zn~(2+)solvation structures in bulk electrolytes,the evolution of interfacial solvation—where Zn~(2+)undergoes desolvation and deposition—remains insufficiently explored.Here,we introduce sulfated nanocellulose(SNC),an anion-rich biopolymer,to tailor the interfacial solvation structure without altering the bulk electrolyte composition.Using in situ attenuated total reflection Fourier transform infrared spectroscopy and fluorescence interface-extended X-ray absorption fine structure,we reveal that SNC facilitates the formation of a low-coordinated Zn~(2+)solvation shell at the interface by weakening H_(2)O coordination.This transformation is driven by electrostatic interactions between Zn~(2+)and anchored sulfate groups,thereby reducing water activity,improving interfacial stability during charge/discharge,and suppressing parasitic reactions.Consequently,a high average coulombic efficiency of 99.6%over 500 cycles in Zn|Ti asymmetric cells and 1.5 Ah pouch cells(13.4 mg cm^(-2)loading,remained stable over 250 cycles)were achieved in SNC-induced AZIBs.This work underscores the importance of interfacial solvation structure engineering—beyond traditional bulk electrolyte design—in enabling practical,high-performance AZIBs.展开更多
Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we d...Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we demonstrate that TSP perovskite films exhibit a vertically gradient distribution of residual PbI_(2)clusters,which form Schottky heterojunctions with the perovskite,leading to substantial interfacial energy-level mismatches within NiO_(x)-based TSP p-i-n PSCs.These limitations were effectively addressed via a vertical interfacial engineering enabled by dual-interface modification incorporating tin trifluoromethanesulfonate(Sn(OTF)_(2))and 4-Fluorophenylethylamine chloride(F-PEA)at the NiO_(x)/perovskite and perovskite/C60 interfaces,respectively.The functional Sn(OTF)_(2)not only enhances the conductivity of NiO_(x)films but also suppresses ion migration,while inducing the formation of a Pb-Sn mixed perovskite interlayer that precisely regulates the energy level at the NiO_(x)/perovskite interface.Complementally,F-PEA post-treatment effectively converts surface residual PbI_(2)clusters into a 2D perovskite capping layer,which simultaneously passivates surface defects and enhances energy-level alignment at the perovskite/C60 interface.Consequently,the optimized NiO_(x)-based TSP p-i-n PSCs achieve a notable PCE of 25.6%with superior operational stability.This study elucidates the underlying mechanisms limiting the efficiency of TSP p-i-n PSCs,while establishing design principles for these devices targeting 26%efficiency.展开更多
Water molecules can form hydrogen bonds.At the solid surfaces,the preferential alignment of water molecules due to the heterogeneous atomic distributions can induce ordered hydrogen bond networks of water molecules wi...Water molecules can form hydrogen bonds.At the solid surfaces,the preferential alignment of water molecules due to the heterogeneous atomic distributions can induce ordered hydrogen bond networks of water molecules with spatially heterogeneous patterns and slower dynamics compared to bulk water.Both the confinement and the surface atomic structures can induce the water phase transitions at low dimensional spaces.Here,we review how the phase transitions of interfacial water affect the surface physical behaviors,such as wetting,ice nucleation and the terahertz-wave-water interactions,from solid materials to the biological surfaces.These works help extend our knowledge of the physics properties of the interfacial water,particularly the multi-phase behaviors in materials and biology sciences.展开更多
The operational temperature rise of photovoltaic(PV)panels reduces their power generation efficiency and shortens their lifespan.Hygroscopic hydrogel-based evaporative cooling technology provides a promising solution ...The operational temperature rise of photovoltaic(PV)panels reduces their power generation efficiency and shortens their lifespan.Hygroscopic hydrogel-based evaporative cooling technology provides a promising solution for PV cooling due to high-enthalpy water evaporation.However,current hydrogels remain plagued by cooling interface mismatch and environmental concerns,which limit their practical implementation.Herein,a“green”and self-adhesive hygroscopic hydrogel consisting only of cheap lotus root powder and LiCl is designed,which can form robust interfacial adhesion with PV panels for efficient and durable cooling.Leveraging its compelling hygroscopicity,the hydrogel is able to rapidly capture moisture to recover cooling capacity,thus achieving self-sustained cooling.Besides,the“salting-in”effect brought by LiCl endows the hydrogel with notable softness and self-adhesiveness,which enables it to tightly combine with PV panels to optimize heat conduction and improve cooling efficiency.As a result,under 1.0 kW m^(-2)illumination,a PV temperature drop of 18.2℃ and a cooling power of 358 W m^(-2)were delivered by attaching the hydrogel to the rear of the PV panel,accompanied by a 7.7%improvement in energy efficiency.Overall,this self-sustained passive cooling strategy,activated by the all-natural hydrogel,sheds light on the development of PV thermal management.展开更多
Interfacial engineering is crucial for developing high-performance Ni-rich layered cathodes for lithiumion batteries.Here,we introduce an interfacial precipitation(IP)strategy,guided by first-principles calculations,t...Interfacial engineering is crucial for developing high-performance Ni-rich layered cathodes for lithiumion batteries.Here,we introduce an interfacial precipitation(IP)strategy,guided by first-principles calculations,to create a functionally graded cathode during precursor synthesis.Based on thermodynamic principles of bulk insolubility and phase separation kinetics,we achieved the selective precipitation of Co onto the surface of a Ni-rich hydroxide precursor.Upon high-temperature lithiation,this engineered precursor spontaneously forms a unique,bifunctional Co-rich spinel-like layer on the final LiNi_(0.88)Co_(0.06)Mn_(0.06)O_(2)(NCM)cathode.This architecture suppresses detrimental Li/Ni cation mixing and protects the active material.Consequently,the IP-driven NCM cathode demonstrates vastly superior rate capability,delivering 140.8 m A h g^(-1)at 5C,compared to 112.9 mA h g^(-1)for its conventionally prepared counterpart.This enhancement is attributed to significantly lower charge-transfer resistance and faster kinetics.Remarkably,in a full-cell configuration,the IP-driven NCM cathode maintains 81.5%capacity after 1000 cycles at an aggressive 5C rate.This work presents a thermodynamically driven,scalable strategy for designing advanced cathodes with exceptional high-power performance and stability.展开更多
Two supramolecular organic frameworks(SOFs)have been constructed from the co-assembly of biimidazolium-derived octacationic components and cucurbit[8]uril in water.Dynamic light scattering and ^(1)H NMR experiments re...Two supramolecular organic frameworks(SOFs)have been constructed from the co-assembly of biimidazolium-derived octacationic components and cucurbit[8]uril in water.Dynamic light scattering and ^(1)H NMR experiments reveal that both SOFs can undergo reversible assembly and disassembly at room temperature.One of the SOFs displays unprecedently high maximum tolerated dose of 120 mg/kg with mice,which improves by 40%compared with the highest value of the reported SOFs.In vitro and in vivo tests show that the SOF can adsorb doxorubicin and overcome the resistance of multidrugresistant MDR A549/ADR tumor cells to realize intracellular delivery,leading to enhanced antitumor efficacy.Moreover,it can also completely inhibit the posttreatment phototoxicity of photofrin and fully neutralize the anticoagulation of both unfractionated heparin and low molecular weight heparins through efficient inclusion and elimination or sequestration mechanism.As the first examples that undergo roomtemperature reversible assembly and disassembly,the new SOFs in principle allow for quantitative analysis of the molecular components in the body that is prerequisite for preclinical evaluation in the future.展开更多
Triclosan(TCS) poses harmful risks to ecosystems and human health owing to its endocrine-disrupting effects.Therefore,developing an efficient and sustainable technology to degrade TCS is urgently needed.Herein,cobalt ...Triclosan(TCS) poses harmful risks to ecosystems and human health owing to its endocrine-disrupting effects.Therefore,developing an efficient and sustainable technology to degrade TCS is urgently needed.Herein,cobalt oxyhydroxide @covalent organic frameworks(CoOOH@COFs) S-scheme heterojunction was synthesized,which combined the visible-light-driven photocatalysis and peroxymonosulfate(PMS) activation to synergistically generate abundant reactive oxygen species(ROSs) for TCS degradation.The degradation efficiency of TCS reached 100 % within 8 min in the Vis-CoOOH@COFs/PMS system,and the reaction rate constant was 0.456 min^(-1),which was nearly 1.90 and 2.85 times that of single Co OOH and COFs,and2.36 times that under dark condition,respectively.The density functional theory(DFT) calculations confirmed the energy band bending of CoOOH@COFs and S-scheme charge transport from COFs to Co OOH.Both experimental and theoretical analyses indicated that Co OOH@COFs in photocatalytic-PMS activation systems synergistically facilitated photo-generated carrier separation,enhanced interfacial electron transfer,accelerated PMS activation,and generated multiple ROSs.In particular,photogenerated electrons(e^(-))accelerated the Co(Ⅲ)/Co(Ⅱ) redox cycle,while the PMS captured the e-,which significantly decreased the charge combination of Co OOH@COFs.Radicals(O_(2)^(·-),^(·)OH,and SO_(4)^(·-)) and non-radicals(such as ^(1)O_(2),h^(+),and e^(-)) were both presented in the Vis-CoOOH@COFs/PMS system,with O_(2)^(-) playing a dominant role in TCS degradation.Furthermore,the pathway of TCS degradation and toxicity of intermediates were explored by DFT calculation and transformation product identification.Importantly,the environmentally friendly CoOOH@COFs S-scheme heterojunction exhibited excellent stability and reusability.In conclusion,this study innovatively designed an S-scheme heterojunction in the photocatalytic-PMS activation system,providing guidance and theoretical support for efficient and eco-friendly wastewater treatment.展开更多
Herein,a reusable and portable surface-enhanced Raman spectroscopy(SERS)sandpaper was successfully synthesized for the sensitive detection of S-fenvalerate in foods.Commercial sandpapers were decorated with Ag@SiO2@Au...Herein,a reusable and portable surface-enhanced Raman spectroscopy(SERS)sandpaper was successfully synthesized for the sensitive detection of S-fenvalerate in foods.Commercial sandpapers were decorated with Ag@SiO2@Au nanoarrays via a liquid-liquid interface self-assembly method.The capacity of sandpaper to float directly on the cyclohexane-water interface allows nanoarrays to be formed directly on it,thereby minimizing stacking issues typically associated with nanoarray assemblies and significantly enhancing the sensitivity of S-fenvalerate detection.Moreover,the SERS sandpaper was reusable and portable due to its strong adhesion of the nanoarrays.Under optimized testing conditions,the developed SERS sandpaper method was capable of detecting S-fenvalerate,demonstrating a strong linear response within a concentration range of 10^(–7)–10^(3)μmol/L,with a limit of detection of 1.92×10^(−8)μmol/L.The analysis of spiked food samples containing S-fenvalerate using the developed SERS sandpaper afforded excellent recoveries(92.2%−109.7%).Additionally,the SERS sandpaper was successfully applied to quantify S-fenvalerate in real food samples,with results consistent with analyses conducted using gas chromatography.展开更多
In coal mining on a high-pressure Ordovician limestone aquifer,grouting materials should have sufficient mechanical properties,particularly strong interfacial bonding performance to address stress concentration at the...In coal mining on a high-pressure Ordovician limestone aquifer,grouting materials should have sufficient mechanical properties,particularly strong interfacial bonding performance to address stress concentration at the grout-limestone interface induced by rock stress disturbances during mining.In this study,graphene oxide(GO)was integrated into cement-polyacrylate composite grout to improve its interfacial bonding.First,four-point bending tests were conducted,and the Monte Carlo method combined with the simplex search algorithm was employed to determine the variations in shear cohesion and static friction parameters.The results reveal that GO can significantly increase both the tensile and shear cohesion of the grout-limestone interface,but minimally affects the interfacial friction coefficient.Second,nuclear magnetic resonance(NMR)and scanning electron microscopy(SEM)tests were performed.The results indicate that GO nanosheets result in a squamaceous microstructure of the grout consolidation mass,increasing the adhesion of the grout-limestone interface.Moreover,spiny Aft(ettringite)clusters can be induced in limestone fracture surfaces by GO,which could serve as anchors for limestone and grout consolidation mass.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funded by the National Research,Development and Inno-vation Office,Hungary(TKP2021-EGA-31,2020-1.1.2-PIACI-KFI-2020-00021,KKP_22 Project no.144180 and FK_23 Project no.146081).Support from Hungarian Research Network(Eötvös Loránd Research Network)grant no.SA-87/2021 and KEP-5/2021 are also acknowledged.Project no.RRF-2.3.1-21-2022-00015+1 种基金supported by the European Union,Recovery and Resilience Facility.The János Bolyai Research Fellowship(A.W.)of the Hungarian Academy of Sciences is greatly acknowledged.The authors acknowledge CF CryoEM of CIISB,Instruct-CZ Centre,supported by Ministry of Education,Youth and Sports,Czech Republic(MEYS CR)(no.LM2023042)European Regional Development Fund-Project"UP CIISB"(n0.CZ.02.1.01/0.0/0.0/18_046/0015974).
文摘Peptide-based assemblies have gained increasing attention in different areas of nanotechnology,drug delivery and molecular biology.Among these,non-natural β-peptide scaffolds are particularly promising,as their programmable and diverse secondary structures,high metabolic stability and strong self-association propensity can be easily exploited to create variable constructs.We have recently demonstrated that heterochiral,acyclic β^(3)-peptides assembled into striped lamellar nanostructures that induced antibacterial activity.The process of this assembly formation could be exploited in diverse areas,however identifying oligomerisation stages,and more importantly,controlling the spontaneous process at different levels is still lacking.In this study,a set of analogues heterochiral hexameric β^(3)-peptide sequences was investigated to understand how systematic,small variations of the sequences,such as single point mutation or N-terminal chemical modification,can influence the resulting assemblies and allow the control of formed morphologies.TEM and cryo-EM combined with molecular dynamics simulation enabled the identification and differentiation of morphological stages throughout the entire multi-step process.Depending on the position of the sequence modifications,the self-assembled structures formed small oligomers,individual protofibrils,extended,flat lamellae,bundles and macroscopic clusters.These results outline how the self-assembly process of short heterochiral β-peptides can be qualitatively fine-tuned by sequence modifications,which contribute to understanding the general peptide assembly processes for their fibrillar morphologies.
基金supported by grants from National Natural Science Foundation of China(224708046,22508229,22278049)Young Elite Scientists Sponsorship Program by CAST(2022QNRC001)+1 种基金Xingliao Talent Program-Young Top Talent(XLYC2403126)Liaoning Provincial Basic Scientific Research Project for Higher Education(LJ212510152013)。
文摘The increasing scarcity of freshwater resources has driven the rapid emergence of solar-driven interfacial evaporators(SDIEs)as a sustainable approach to harvest fresh water by utilizing solar energy.Lignocellulosic biomass,featuring natural abundance,excellent renewability,unique natural structures,and superior biodegradability compared to the synthetic polymers,is highly attractive for constructing solar steam generators.This review aims to offer an innovative and in-depth insight into designing and optimizing highperformance integrated solar interfacial evaporators derived from renewable lignocellulosic biomass.First,the structural characteristics of lignocellulosic biomass are briefly introduced,serving as photothermal layer or supporting substrates in SDIEs.Secondly,the fabrication methods and processing technologies of lignocellulosic biomass-based evaporators are summarized from the perspective of photothermal layer and supporting substrates.Next,the most recent advances of regulation and optimization strategies are proposed to improve evaporation efficiency.Subsequently,this review summarizes the diverse functionalities of SDIEs,including desalination,power generation,wastewater treatment and antimicrobial,atmospheric water harvesting,and photocatalytic hydrogen production.Finally,the challenges in this field and outlook on the future development are discussed,which are anticipated to provide new opportunities for the advancement of lignocellulosic biomass-based SDIEs.
基金the research grant from the Youth Fund of the National Natural Science Foundation of China(62305340)the financial support from the Hong Kong Research Grant Council via STEM Postdoctoral Fellowship(Project no.9446002)+6 种基金the Alexander von Humboldt Foundation and the support during his stay in Christoph J.Brabec’s group at Friedrich-Alexander-Universität Erlangen-Nürnberg and Helmholtz-Institute Erlangen-Nürnberg(HI ERN)the research grant from KAUST global fellowship postdocfinancial support from the Innovation and Technology Commission(Grant no.MHP/104/21)Shenzhen Science and Technology Innovation Commission(JCYJ20210324125612035,R-IND12303,and R-IND12304)the National Key Research and Development Program of China(no.2021YFA1500900)the National Natural Science Foundation of China(no.52071174)the support from the Hong Kong Jockey Club under the research work Hong Kong JC STEM Lab for Circular Bio-economy(Project No.2023-0078)。
文摘Sustainability and scalability remain critical hurdles for the commercialization of organic solar cells(OSCs).However,addressing both poses challenge.Herein,we introduce a simple yet effective strategy utilizing 3,5-dichloropyridine(PDCC)as a solid additive to fine-tune the self-assembly behavior of Y-series non-fullerene acceptors(NFAs)to tackle the upscaling limitations in green-solvent-processed OSCs.PDCC predominantly interacts with Y-series NFAs,facilitating molecular crystallization and thereby driving the self-assembly of Y-series NFAs during film-forming dynamics,leading to more uniform active layers with improved molecular packing and reduced charge recombination.As a result,PDCC-driven self-assembly strategy enables high-performance OSCs with a power conversion efficiency(PCE)of 20.47%.When translated to sustainable fabrication,this strategy significantly boosts the PCE of large-area green-solvent-processed OSC modules(19.3 cm^(2))from 13.87%to 15.79%,ranking it among the best-performing green-solvent-processed large-area OSC modules(>18 cm^(2)).Beyond its impact on PCE enhancement,PDCC serves as a multifunctional additive to improve long-term stability and exhibits strong universality across multiple material systems.This work establishes a promising approach for advancing sustainable and scalable OSCs,paving the way for their commercialization.
基金supported by the National Natural Science Foundation of China(32571991)Guangxi Natural Science Foundation of China(2023GXNSFGA026001&2025GXNSFAA069870)the Foundation of State Key Laboratory of Biobased Material and Green Papermaking.(No.GZKF202323)。
文摘The rapid advancement of flexible electronics technology has placed higher demands on the structural design and performance regulation of elastic materials.Cellulosic elastomers,with their biodegradability,renewability,and tunability,emerge as ideal candidate materials.Entropy-driven self-as sembly promotes the spontaneous formation of ordered structures,serving as a crucial pathway for optimizing cellulose elastomer properties.However,the structure-property relationship between the self-assembled ordered structures of cellulose elastomers and their mechanical and electrical properties remains insufficiently explored.It hinders the expansion of their applications in electronic devices.This paper systematically reviews the structure-property regulation mechanisms of self-assembled cellulosic elastomers from an entropy-driven perspective.It elucidates the application principles and performance optimization strategies for mechanical energy harvesting and self-powered sensing,while also exploring the challenges and prospects for performance enhancement.This work provides a reference for the development of self-assembled cellulosic elastomers in the field of energy devices.
基金financially supported by the Fundamental Research Funds for Central Universities(No.24D110627)。
文摘The preparation and functionalization of polymeric capsules attract intense attention due to their application in various areas.Herein we presented an amphiphilic alternating copolymer(ACP)-based microcapsule which is both robust and readily-functionalized through interfacial click polymerization.A water-in-oil emulsion was constructed to act as the reaction medium,the hydrophilic 1,3-butadiene diepoxide(BDE)in water phase reacted with the oleophilic 1,4-dibutanedithiol(BDT)in oil phase at the water-oil interface to form the amphiphilic ACP named poly(2,3-dihydroxy butylene-alt-butylene dithioether)(abbreviated as P(DHB-a-BDT)below),which would deposite in situ to form the micro-sized capsules.Significantly,the dried capsules are robust enough to be rehydrated once the water was added and almost restored their original morphologies.Further elucidation showed that the Young's modulus of these capsules exceeded 1 GPa.As long as we know,it is the first time for the mechanical properties of the ACP-based microstructures being investigated.Besides,functionalization could be achieved simultaneously with the formation process.As a proof of concept,positive-charged capsules were successfully obtained through click copolymerization.Stemming from the unique characteristics of amphiphilic ACPs which combined both merits of click chemistry and interfacial reactions,all these features of the current method as well as the resultant capsules may promote the application of the polymeric capsules.
文摘Peroxymonosulfate(PMS)-assisted visible-light photocatalytic degradation of organic pollutants using graphitic carbon nitride(g-C_(3)N_(4))presents a promising and environmentally friendly approach.However,pristine g-C_(3)N_(4) suffers from limited visible-light absorption and low charge-carrier mobility.In this study,a phosphorus-doped tubular carbon nitride(5P-TCN)was synthesized via a precursor self-assembly method using phosphoric acid and melamine as raw materials,eliminating the need for organic solvents or templates.The 5P-TCN catalyst demonstrated enhanced visible-light absorption,improved charge transfer capability,and a 5.25-fold increase in specific surface area(31.092 m^(2)/g),which provided abundant active sites to efficiently drive the PMS-assisted photocatalytic reaction.The 5P-TCN/vis/PMS system exhibited exceptional degradation performance for organic pollutants across a broad pH range(3–9),achieving over 92%degradation of Rhodamine B(RhB)within 15 min.Notably,the system retained>98%RhB degradation efficiency after three consecutive operational cycles,demonstrating robust operational stability and reusability.Moreover,key parameters influencing,active radi-cals,degradation pathways,and potential mechanisms for RhB degradation were systematically investigated.This work proposes a green and cost-effective strategy for developing high-efficiency photocatalysts,while demon-strating the exceptional capability of a PMS-assisted photocatalytic system for rapid degradation of RhB.
基金supported by the fund of State Key Laboratory of Clean and Efficient Turbomachinery Power Equipment(No.DEC8300CG202210353EE280297)the China Postdoctoral Science Foundation(No.2021M692555)+1 种基金the Shaanxi Province Qinchuangyuan‘Scientists+Engineers’Team Building Project(No.2023KXJ-266)the Fundamental Research Funds for the Central Universities(No.xzy012023145)。
文摘Low reactivity and appropriate wettability between molten superalloys and ceramic materials are crucial for the production of high-quality superalloy castings.The sessile-drop experiment was employed to systematically investigate the interfacial reaction and wettability between the 4777DS1 superalloy and SiO_(2)-based ceramic core at various temperatures(1,480℃,1,500℃,1,520℃,and 1,550℃).The wetting behavior and interfacial reaction products at different temperatures were analyzed by scanning electron microscopy(SEM),energy dispersive spectroscopy(EDS),and X-ray diffraction(XRD).The interfacial reaction process and products were discussed,and the thermodynamic behavior and interfacial reaction mechanisms were elucidated.The results demonstrate that the wetting behavior and interfacial reaction between the 4777DS1 alloy and the ceramic core are significantly influenced by temperature.The wettability angle exhibits a trend of initial decrease followed by an increase with rising temperature,reaching a maximum of 139°at 1,480℃,indicating poorer wettability of the 4777DS1 superalloy with the ceramic core and better casting properties at this specific temperature.The most intense interfacial reaction occurs at 1,520℃,resulting in the formation of the main interfacial reaction products such as Al_(2)O_(3),SiO_(2),and HfO_(2).Additionally,some crystal-like products rich in Si and Hf distribute on the reaction layer.
基金financial support of the National Natural Science Foundation of China(Nos.62464011,62474084,52462025)Natural Science Foundation of Jiangxi Province(No.20242BAB25226)。
文摘Understanding the intricate interplay between electrode reactivity and interfacial chemistry is crucial for advancing halide perovskite memristors toward practical applications.Here,we systematically investigate how top electrode materials(Au,Ag,Cu,Al)influence the resistive switching behavior of quasi-2D CsPbBr_(3) devices through controlled interfacial engineering.By introducing a novel bilayer electrode architecture,we successfully decouple electrode surface oxidation effects from perovskite/electrode interfacial oxidation reactions for the first time.In situ XRD,photoluminescence spectroscopy,and interfacial XPS analysis reveal that voltage-driven bromide ion migration coupled with electrode-dependent reactions governs the switching mechanisms.Chemically inert Au electrodes show no switching due to insufficient interfacial reactivity,while highly reactive Al electrodes cause irreversible degradation through excessive chemical interactions.In contrast,moderately active Ag and Cu electrodes enable stable bipolar switching with dual negative differential resistance characteristics.The optimal performance emerges from balanced electrode reactivity that facilitates reversible interfacial redox reactions without structural degradation.These findings establish fundamental design principles linking electrode chemical activity to device functionality,providing a rational framework for engineering robust perovskite memristors with enhanced stability and performance for next-generation memory and neuromorphic computing applications.
文摘To develop specific lining materials for rare earth steel nozzles,LaAlO_(3)powder was first synthesized by high-temperature solid-phase synthesis at 1400℃for 3 h using La_(2)O_(3)and Al_(2)O_(3)powders as raw materials.Then BN,AlN,Si_(3)N_(4)and TiN powders were pressed intoφ30 mm×7 mm substrate samples under 120 MPa with PVA as the binder.Equal amounts of La_(2)O_(3)and LaAlO_(3)powders were placed on their surfaces,reacting at 1550℃for 3 h in different atmospheres(reducing and argon conditions).The interfacial reactions of the four nitride(BN,Si_(3)N_(4),AlN,and TiN)substrate samples with La_(2)O_(3)and LaAlO_(3)in different atmospheres were studied,respectively.The results show that in reducing and argon atmospheres,the intensity order of the reactions between the four nitrides and La_(2)O_(3)is Si_(3)N_(4)>BN>AlN>TiN.In the reducing atmosphere,the reaction intensity order of the four nitrides with LaAlO_(3)is Si_(3)N_(4)>AlN≈TiN>BN.However,in the argon atmosphere,the order is Si_(3)N_(4)>BN>AlN≈TiN.TiN has good structural stability in both reducing and argon atmospheres,and shows weak reactivity with La_(2)O_(3)and LaAlO_(3).It is a relatively good anti-clogging lining material for rare earth steel nozzles.
基金supported by the National Natural Science Foundation of China(No.22278156)the Guangdong Special Support Program Project(No.2021JC060580)+1 种基金the Young Elite Scientists Sponsorship Program by CAST-Doctoral Student Special Plan,the China Scholarship Council Program(No.202406150148)the Natural Science Foundation of Guangdong Province(No.2023A1515011186).
文摘Peroxymonosulfate(PMS)-based advanced oxidation processes(AOPs)are an effective way to remove emerging contaminants(ECs)from water.The catalytic process involving PMS is hindered by the suboptimal electron trans-fer efficiency of current catalysts,the further application of AOPs technology is limited.Here,it is proposed that the interfacial electric field can be controlled by bor(B)-doped FeNC catalysts,which shows significant advantages in the efficient generation,release and participation of reactive oxygen species(ROS)in the reaction.The super exchange interaction between Fe sites and N and B sites is realized through the directional transfer of electrons in the interfacial electric field,which ensures the high efficiency and stability of the PMS catalytic process.B doping increases the d orbitals distribution at Fermi level,which facilitates enhanced electron transition activity,thereby promoting the effective generation of (1)^O_(2).At the same time,orbital hybridization causes the center of the d band to move to a lower energy level,which not only contributes to the desorption process of (1)^O_(2),but also accelerates its release.In addition,B-doping also improved the adsorption capacity of organic pollutants and shortened the migration distance of ROS,thereby significantly improving the degradation efficiency of ECs.The B-doping strategy outlined offers a novel approach to the development of FeNC catalysts,it lays a theoretical foundation and offers technical insights for the integration of PMS/AOPs technology in the ECs management.
基金the National Natural Science Foundation of China(No.22379047)Yinzhou R&D Team(X.W.)+2 种基金Guangdong Basic and Applied Basic Research Foundation(2022B1515120019)the Project Funded by the China Scholarship Council(No.202108320278)the support from the Vacuum Interconnected Nanotech Workstation(Nano-X)from Suzhou Institute of Nano-Tech and Nano-Bionics,Chinese Academy of Sciences(SINANO)。
文摘Aqueous zinc-ion batteries(AZIBs)offer a safe,cost-effective,and high-capacity energy storage solution,yet their performance is hindered by interfacial challenges at the Zn anode,including hydrogen evolution,corrosion,and dendritic Zn growth.While most studies focus on regulating Zn~(2+)solvation structures in bulk electrolytes,the evolution of interfacial solvation—where Zn~(2+)undergoes desolvation and deposition—remains insufficiently explored.Here,we introduce sulfated nanocellulose(SNC),an anion-rich biopolymer,to tailor the interfacial solvation structure without altering the bulk electrolyte composition.Using in situ attenuated total reflection Fourier transform infrared spectroscopy and fluorescence interface-extended X-ray absorption fine structure,we reveal that SNC facilitates the formation of a low-coordinated Zn~(2+)solvation shell at the interface by weakening H_(2)O coordination.This transformation is driven by electrostatic interactions between Zn~(2+)and anchored sulfate groups,thereby reducing water activity,improving interfacial stability during charge/discharge,and suppressing parasitic reactions.Consequently,a high average coulombic efficiency of 99.6%over 500 cycles in Zn|Ti asymmetric cells and 1.5 Ah pouch cells(13.4 mg cm^(-2)loading,remained stable over 250 cycles)were achieved in SNC-induced AZIBs.This work underscores the importance of interfacial solvation structure engineering—beyond traditional bulk electrolyte design—in enabling practical,high-performance AZIBs.
基金financially supported by the National Nature Science Foundation of China (62504130)National Key Research and Development Program of China (2018YFB0704100)+3 种基金the Key university laboratory of highly efficient utilization of solar energy and sustainable development of Guangdong (Y01256331)the Technology Development Project of Henan Province (252102240047)the Pico Center at SUSTech CRF which receives support from the Presidential FundDevelopment and Reform Commission of Shenzhen Municipality
文摘Two-step-processed(TSP)inverted p-i-n perovskite solar cells(PSCs)have demonstrated significant promise in tandem applications.However,the power conversion efficiency(PCE)of TSP p-i-n PSCs rarely exceeds 24%.Here,we demonstrate that TSP perovskite films exhibit a vertically gradient distribution of residual PbI_(2)clusters,which form Schottky heterojunctions with the perovskite,leading to substantial interfacial energy-level mismatches within NiO_(x)-based TSP p-i-n PSCs.These limitations were effectively addressed via a vertical interfacial engineering enabled by dual-interface modification incorporating tin trifluoromethanesulfonate(Sn(OTF)_(2))and 4-Fluorophenylethylamine chloride(F-PEA)at the NiO_(x)/perovskite and perovskite/C60 interfaces,respectively.The functional Sn(OTF)_(2)not only enhances the conductivity of NiO_(x)films but also suppresses ion migration,while inducing the formation of a Pb-Sn mixed perovskite interlayer that precisely regulates the energy level at the NiO_(x)/perovskite interface.Complementally,F-PEA post-treatment effectively converts surface residual PbI_(2)clusters into a 2D perovskite capping layer,which simultaneously passivates surface defects and enhances energy-level alignment at the perovskite/C60 interface.Consequently,the optimized NiO_(x)-based TSP p-i-n PSCs achieve a notable PCE of 25.6%with superior operational stability.This study elucidates the underlying mechanisms limiting the efficiency of TSP p-i-n PSCs,while establishing design principles for these devices targeting 26%efficiency.
基金supported by the National Natural Science Foundation of China(Grant Nos.22576126,12074394,12022508).
文摘Water molecules can form hydrogen bonds.At the solid surfaces,the preferential alignment of water molecules due to the heterogeneous atomic distributions can induce ordered hydrogen bond networks of water molecules with spatially heterogeneous patterns and slower dynamics compared to bulk water.Both the confinement and the surface atomic structures can induce the water phase transitions at low dimensional spaces.Here,we review how the phase transitions of interfacial water affect the surface physical behaviors,such as wetting,ice nucleation and the terahertz-wave-water interactions,from solid materials to the biological surfaces.These works help extend our knowledge of the physics properties of the interfacial water,particularly the multi-phase behaviors in materials and biology sciences.
基金supported by the National Natural Science Foundation of China(52473033)。
文摘The operational temperature rise of photovoltaic(PV)panels reduces their power generation efficiency and shortens their lifespan.Hygroscopic hydrogel-based evaporative cooling technology provides a promising solution for PV cooling due to high-enthalpy water evaporation.However,current hydrogels remain plagued by cooling interface mismatch and environmental concerns,which limit their practical implementation.Herein,a“green”and self-adhesive hygroscopic hydrogel consisting only of cheap lotus root powder and LiCl is designed,which can form robust interfacial adhesion with PV panels for efficient and durable cooling.Leveraging its compelling hygroscopicity,the hydrogel is able to rapidly capture moisture to recover cooling capacity,thus achieving self-sustained cooling.Besides,the“salting-in”effect brought by LiCl endows the hydrogel with notable softness and self-adhesiveness,which enables it to tightly combine with PV panels to optimize heat conduction and improve cooling efficiency.As a result,under 1.0 kW m^(-2)illumination,a PV temperature drop of 18.2℃ and a cooling power of 358 W m^(-2)were delivered by attaching the hydrogel to the rear of the PV panel,accompanied by a 7.7%improvement in energy efficiency.Overall,this self-sustained passive cooling strategy,activated by the all-natural hydrogel,sheds light on the development of PV thermal management.
基金supported by grants from the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(MSIT)(RS-2024-00407116)+1 种基金by the Ministry of Education(NRF-2018R1A6A1A03024231)support from the NRF grant funded by the MSIT(RS-2024-00406724)。
文摘Interfacial engineering is crucial for developing high-performance Ni-rich layered cathodes for lithiumion batteries.Here,we introduce an interfacial precipitation(IP)strategy,guided by first-principles calculations,to create a functionally graded cathode during precursor synthesis.Based on thermodynamic principles of bulk insolubility and phase separation kinetics,we achieved the selective precipitation of Co onto the surface of a Ni-rich hydroxide precursor.Upon high-temperature lithiation,this engineered precursor spontaneously forms a unique,bifunctional Co-rich spinel-like layer on the final LiNi_(0.88)Co_(0.06)Mn_(0.06)O_(2)(NCM)cathode.This architecture suppresses detrimental Li/Ni cation mixing and protects the active material.Consequently,the IP-driven NCM cathode demonstrates vastly superior rate capability,delivering 140.8 m A h g^(-1)at 5C,compared to 112.9 mA h g^(-1)for its conventionally prepared counterpart.This enhancement is attributed to significantly lower charge-transfer resistance and faster kinetics.Remarkably,in a full-cell configuration,the IP-driven NCM cathode maintains 81.5%capacity after 1000 cycles at an aggressive 5C rate.This work presents a thermodynamically driven,scalable strategy for designing advanced cathodes with exceptional high-power performance and stability.
基金the National Natural Science Foundation of China(No.21921003 for Z.T.L.and 22201293 for S.B.Y.)Shanghai Sailing Program(No.22YF1458300 for S.B.Y.)for financial support。
文摘Two supramolecular organic frameworks(SOFs)have been constructed from the co-assembly of biimidazolium-derived octacationic components and cucurbit[8]uril in water.Dynamic light scattering and ^(1)H NMR experiments reveal that both SOFs can undergo reversible assembly and disassembly at room temperature.One of the SOFs displays unprecedently high maximum tolerated dose of 120 mg/kg with mice,which improves by 40%compared with the highest value of the reported SOFs.In vitro and in vivo tests show that the SOF can adsorb doxorubicin and overcome the resistance of multidrugresistant MDR A549/ADR tumor cells to realize intracellular delivery,leading to enhanced antitumor efficacy.Moreover,it can also completely inhibit the posttreatment phototoxicity of photofrin and fully neutralize the anticoagulation of both unfractionated heparin and low molecular weight heparins through efficient inclusion and elimination or sequestration mechanism.As the first examples that undergo roomtemperature reversible assembly and disassembly,the new SOFs in principle allow for quantitative analysis of the molecular components in the body that is prerequisite for preclinical evaluation in the future.
文摘Triclosan(TCS) poses harmful risks to ecosystems and human health owing to its endocrine-disrupting effects.Therefore,developing an efficient and sustainable technology to degrade TCS is urgently needed.Herein,cobalt oxyhydroxide @covalent organic frameworks(CoOOH@COFs) S-scheme heterojunction was synthesized,which combined the visible-light-driven photocatalysis and peroxymonosulfate(PMS) activation to synergistically generate abundant reactive oxygen species(ROSs) for TCS degradation.The degradation efficiency of TCS reached 100 % within 8 min in the Vis-CoOOH@COFs/PMS system,and the reaction rate constant was 0.456 min^(-1),which was nearly 1.90 and 2.85 times that of single Co OOH and COFs,and2.36 times that under dark condition,respectively.The density functional theory(DFT) calculations confirmed the energy band bending of CoOOH@COFs and S-scheme charge transport from COFs to Co OOH.Both experimental and theoretical analyses indicated that Co OOH@COFs in photocatalytic-PMS activation systems synergistically facilitated photo-generated carrier separation,enhanced interfacial electron transfer,accelerated PMS activation,and generated multiple ROSs.In particular,photogenerated electrons(e^(-))accelerated the Co(Ⅲ)/Co(Ⅱ) redox cycle,while the PMS captured the e-,which significantly decreased the charge combination of Co OOH@COFs.Radicals(O_(2)^(·-),^(·)OH,and SO_(4)^(·-)) and non-radicals(such as ^(1)O_(2),h^(+),and e^(-)) were both presented in the Vis-CoOOH@COFs/PMS system,with O_(2)^(-) playing a dominant role in TCS degradation.Furthermore,the pathway of TCS degradation and toxicity of intermediates were explored by DFT calculation and transformation product identification.Importantly,the environmentally friendly CoOOH@COFs S-scheme heterojunction exhibited excellent stability and reusability.In conclusion,this study innovatively designed an S-scheme heterojunction in the photocatalytic-PMS activation system,providing guidance and theoretical support for efficient and eco-friendly wastewater treatment.
基金financially supported by the Key R&D Program of Shandong Province,China(2023CXGC010712).
文摘Herein,a reusable and portable surface-enhanced Raman spectroscopy(SERS)sandpaper was successfully synthesized for the sensitive detection of S-fenvalerate in foods.Commercial sandpapers were decorated with Ag@SiO2@Au nanoarrays via a liquid-liquid interface self-assembly method.The capacity of sandpaper to float directly on the cyclohexane-water interface allows nanoarrays to be formed directly on it,thereby minimizing stacking issues typically associated with nanoarray assemblies and significantly enhancing the sensitivity of S-fenvalerate detection.Moreover,the SERS sandpaper was reusable and portable due to its strong adhesion of the nanoarrays.Under optimized testing conditions,the developed SERS sandpaper method was capable of detecting S-fenvalerate,demonstrating a strong linear response within a concentration range of 10^(–7)–10^(3)μmol/L,with a limit of detection of 1.92×10^(−8)μmol/L.The analysis of spiked food samples containing S-fenvalerate using the developed SERS sandpaper afforded excellent recoveries(92.2%−109.7%).Additionally,the SERS sandpaper was successfully applied to quantify S-fenvalerate in real food samples,with results consistent with analyses conducted using gas chromatography.
基金supported by the National Key R&D Program of China(Grant Nos.U25A20810 and 2024YFF0508201)the National Natural Science Foundation of China(Grant No.12302504).
文摘In coal mining on a high-pressure Ordovician limestone aquifer,grouting materials should have sufficient mechanical properties,particularly strong interfacial bonding performance to address stress concentration at the grout-limestone interface induced by rock stress disturbances during mining.In this study,graphene oxide(GO)was integrated into cement-polyacrylate composite grout to improve its interfacial bonding.First,four-point bending tests were conducted,and the Monte Carlo method combined with the simplex search algorithm was employed to determine the variations in shear cohesion and static friction parameters.The results reveal that GO can significantly increase both the tensile and shear cohesion of the grout-limestone interface,but minimally affects the interfacial friction coefficient.Second,nuclear magnetic resonance(NMR)and scanning electron microscopy(SEM)tests were performed.The results indicate that GO nanosheets result in a squamaceous microstructure of the grout consolidation mass,increasing the adhesion of the grout-limestone interface.Moreover,spiny Aft(ettringite)clusters can be induced in limestone fracture surfaces by GO,which could serve as anchors for limestone and grout consolidation mass.