Entropy is a basic thermodynamic property of the electrical double layer(EDL)at metal/solution interfaces,yet,its definition,measurement,and theoretical treatment are dispersed in the literature,and,in some cases,ambi...Entropy is a basic thermodynamic property of the electrical double layer(EDL)at metal/solution interfaces,yet,its definition,measurement,and theoretical treatment are dispersed in the literature,and,in some cases,ambiguous.In this paper,we revisit the thermodynamic theory of EDL,from which two variants of entropy,excess entropy and formation entropy,are obtained and compared.In terms of the formation entropy,two calculation routes are validated in the context of a primitive EDL model,namely,the Gouy-Chapman(GC)model.After clarifying the concepts and calculation routes,we investigate interfacial water effects on the EDL entropy,using a refined Gouy-Chapman-Stern(GCS)model accounting for chemical potential difference between oxygen-and hydrogen-down water molecules,denotedδμ.The model-derived differential capacitance and entropy are compared with experimental data for the EDL at Au(111)in an aqueous electrolyte solution.The model reveals that the charge of maximum entropy(CME)is negative when water molecules have higher tendency to take oxygen-down configuration at the uncharged surface.Moreover,the formation entropy profile becomes asymmetric around the CME,whenδμis potential-dependent.However,the model fails to simultaneously reproduce capacitance and entropy measurements on the same system taken from two separate studies,indicating deficiencies of the model or experimental errors.Nevertheless,this work stresses the importance of measuring both capacitance and entropy of EDLs at the same time.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 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
The interfacial properties of steel-mushy Al-28Pb bonding plate with different interfacial structures, and the influence of ratio of Fe-Al compound at the interface on interfacial shear strength were investigated. The...The interfacial properties of steel-mushy Al-28Pb bonding plate with different interfacial structures, and the influence of ratio of Fe-Al compound at the interface on interfacial shear strength were investigated. The results show that there is a nonlinear relationship between the ratio of Fe-Al compound at the interface and the interfacial shear strength. When the ratio of Fe-Al compound at the interface is smaller than 71.4%, with the increase of the ratio of Fe-Al compound at the interface, the interfacial shear strength increases gradually; when the ratio of Fe-Al compound at the interface is larger than 71.4%, with the increase of the ratio of Fe-Al compound at the interface, the interfacial shear strength decreases continuously; when the ratio of Fe-Al compound at the interface is 71.4%, the largest interfacial shear strength 70.2MPa is obtained.展开更多
The interface properties between hydrated cement paste(hcp)and aggregates largely determine the various performances of concrete.In this work,molecular dynamics simulations were employed to explore the atomistic inter...The interface properties between hydrated cement paste(hcp)and aggregates largely determine the various performances of concrete.In this work,molecular dynamics simulations were employed to explore the atomistic interaction mechanisms between the commonly used aggregate phase calcite/silica and calcium silicate hydrates(C-S-H),as well as the effect of moisture.The results suggest that the C-S-H/calcite interface is relatively strong and stable under both dry and moist conditions,which is caused by the high-strength interfacial connections formed between calcium ions from calcite and high-polarity non-bridging oxygen atoms from the C-S-H surface.Silica can be also adsorbed on the dry C-S-H surface by the H-bonds;however,the presence of water molecules on the interface may substantially decrease the affinities.Furthermore,the dynamics interface separation tests of C-S-H/aggregates were also implemented by molecular dynamics.The shape of the calculated stress-separation distance curves obeys the quasi-static cohesive law obtained experimentally.The moisture conditions and strain rates were found to affect the separation process of C-S-H/silica.A wetter interface and smaller loading rate may lead to a lower adhesion strength.The mechanisms interpreted here may shed new lights on the understandings of hcp/aggregate interactions at a nano-length scale and creation of high performance cementitious materials.展开更多
The hydration film on particle surface plays an important role in bubble-particle adhesion in mineral flotation process. The thicknesses of the hydration films on natural hydrophobic coal and hydrophilic mica surfaces...The hydration film on particle surface plays an important role in bubble-particle adhesion in mineral flotation process. The thicknesses of the hydration films on natural hydrophobic coal and hydrophilic mica surfaces were measured directly by atomic force microscopy (AFM) based on the bending mode of the nominal constant compliance regime in AFM force curve in the present study. Surface and solid-liquid interfacial energies were calculated to explain the forming mechanism of the hydration film and atomic force microscopy data. The results show that there are significant differences in the structure and thickness of hydration films on coal and mica surfaces. Hydration film formed on mica surface with the thickness of 22.5 nm. In contrast, the bend was not detected in the nominal constant compliance regime. The van der Waals and polar interactions between both mica and coal and water molecules are characterized by an attractive effect, while the polar attractive free energy between water and mica (-87.36 mN/m) is significantly larger than that between water and coal (-32.89 mN/m), which leads to a thicker and firmer hydration layer on the mica surface. The interfacial interaction free energy of the coal/water/bubble is greater than that of mica. The polar attractive force is large enough to overcome the repulsive van der Waals force and the low energy barrier of film rupture, achieving coal particle bubble adhesion with a total interfacial free energy of-56.30 mN/m.展开更多
A series of In_(x)Sb_(2-x)S_(3) nanosheets modified g-C_(3)N_(4)(In_(x)Sb_(2-x)S_(3)-TCN)heterojunctions with different g-C_(3)N_(4) contents were fabricated by an in situ deposition method.All the In_(x)Sb_(2-x)S_(3)...A series of In_(x)Sb_(2-x)S_(3) nanosheets modified g-C_(3)N_(4)(In_(x)Sb_(2-x)S_(3)-TCN)heterojunctions with different g-C_(3)N_(4) contents were fabricated by an in situ deposition method.All the In_(x)Sb_(2-x)S_(3)-TCN composites were applied as photocatalysts in Cr(Ⅵ)polluted water treatment and the results displayed that In_(x)Sb_(2-x)S_(3)-TCN could effectively remove Cr(Ⅵ)under visible light through synergistic effects of adsorption and photocatalytic reduction.Especially,In_(x)Sb_(2-x)S_(3)-TCN-70(70 mg g-C_(3)N_(4)) exhibited the most excellent adsorption and photocatalytic reduction performance among all composites,which possessed a high equilibrium adsorption capacity of 12.45 mg/g in a 30.0 mg/L Cr(Ⅵ)aqueous solution,and reduced Cr(Ⅵ)to Cr(Ⅲ)within 10 min under visible light irradiation.DRS and PL results indicated that the interfacial coupling effect between g-C_(3)N_(4)and In_(x)Sb_(2-x)S_(3) enhanced the utilization efficiency of visible light and suppressed photoinduced carrier recombination,which improved the photocatalytic activity of composites.Moreover,the photocatalyst exhibited satisfactory reduction activity and good stability after 5 cycles of Cr(Ⅵ)adsorptionphotoreduction.展开更多
Rapidly solidified Sn-9Zn-0.1Pr(/Nd) alloy foils were prepared by melt-spinning method. Through comparison, the effects of rapid solidification process and 0.1%Pr/Nd(mass fraction) addition on the microstructure, ther...Rapidly solidified Sn-9Zn-0.1Pr(/Nd) alloy foils were prepared by melt-spinning method. Through comparison, the effects of rapid solidification process and 0.1%Pr/Nd(mass fraction) addition on the microstructure, thermodynamic characteristic of Sn-9Zn solder alloy were analyzed. The tensile-shear tests were used to evaluate the mechanical properties of solder/Cu joints. The results show that the rapid solidification process can greatly refine the microstructure of Sn-9Zn-0.1Pr(/Nd) alloys. After rapid solidification, the effects of Pr/Nd addition on microstructure are depressed. The pasty range of the rapidly solidified Sn-Zn-RE solders is also reduced significantly. The mechanical properties of solder/Cu joints are obviously improved using the rapidly solidified Sn-9Zn-0.1Pr(/Nd) solder alloy, which results in the formation of uniform interface. The promotion effect of Nd addition in Sn-9Zn alloy on the interfacial reaction of solder/Cu joint is more remarkable than that of Pr.展开更多
The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves...The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves the pretreatment of HMX to endow—OH groups on the surface via polyalcohol bonding agent modification and in situ coating with nitrate ester-containing polymer,was proposed to address the problem.Two types of energetic polyether—glycidyl azide polymer(GAP)and nitrate modified GAP(GNP)were grafted onto HMX crystal based on isocyanate addition reaction bridged through neutral polymeric bonding agent(NPBA)layer.The morphology and structure of the HMX-based composites were characterized in detail and the core-shell structure was validated.The grafted polymers obviously enhanced the adhesion force between HMX crystals and fluoropolymer(F2314)binder.Due to the interfacial reinforcement among the components,the two HMX-based composites exhibited a remarkable increment of phase transition peak temperature by 10.2°C and 19.6°C with no more than 1.5%shell content,respectively.Furthermore,the impact and friction sensitivity of the composites decreased significantly as a result of the barrier produced by the grafted polymers.These findings will enhance the future prospects for the interface design of energetic composites aiming to solve the weak interface and safety concerns.展开更多
The organic phase separated from the interfacial crud provided by Dexing copper mine in Jiangxi, China, was analyzed by combined gas chromatography-mass spectroscopy. The results show that many kinds of emphiphiles co...The organic phase separated from the interfacial crud provided by Dexing copper mine in Jiangxi, China, was analyzed by combined gas chromatography-mass spectroscopy. The results show that many kinds of emphiphiles containing such hydrophilic groups as carbonyl, carboxyl, sulphonyl or acylamine exist in organic phase. Conclusively, Lix984N would degrade gradually during a long-term contact with the acidic aqueous feed and strip reagents. Lix84 and nonylphenol as effective components of Lix984N degraded almost completely after long-term recycling. Lix984N degraded through such reactions as Beck.mann rearrange, hydrolysis and sulphofication. The degradation of Lix984N would deteriorate solvent extraction and disengagement performance, and result in a more stable interracial emulsion.展开更多
H+ doped polyaniline nanofibre(PH) was synthesized by interfacial polymerization and polyanilines doped with Li salt(PLI and PHLI) were prepared by immersing emeraldine base(EB) and H+ doped polyaniline in 1 mol/L LiP...H+ doped polyaniline nanofibre(PH) was synthesized by interfacial polymerization and polyanilines doped with Li salt(PLI and PHLI) were prepared by immersing emeraldine base(EB) and H+ doped polyaniline in 1 mol/L LiPF6/(EC-EMC-DMC),respectively.PH,PLI and PHLI were all characterized by scanning electron microscopy(SEM) and Fourier transform infrared(FT-IR) spectrometry.With 1 mol/L LiPF6/(EC-EMC-DMC) as electrolyte,PH,PHLI and PLI were used as the active materials of symmetric non-aqueous redox supercapacitors.PLI shows the highest initial specific capacitance of 120 F/g(47 F/g for PH and 66 F/g for PHLI) among three samples.After 500 cycles,the specific capacitance of PLI remains 75 F/g,indicating the good cycleability.展开更多
Numerical simulations based on a new regularized phase-field model were presented, to simulate the solidification of hexagonal close-packed materials with strong interfacial energy anisotropies. Results show that the ...Numerical simulations based on a new regularized phase-field model were presented, to simulate the solidification of hexagonal close-packed materials with strong interfacial energy anisotropies. Results show that the crystal grows into facet dendrites,displaying six-fold symmetry. The size of initial crystals has an effect on the branching-off of the principal branch tip along the<100> direction, which is eliminated by setting the b/a(a and b are the semi-major and semi-minor sizes in the initial elliptical crystals, respectively) value to be less than or equal to 1. With an increase in the undercooling value, the equilibrium morphology of the crystal changes from a star-like shape to facet dendrites without side branches. The steady-state tip velocity increases exponentially when the dimensionless undercooling is below the critical value. With a further increase in the undercooling value, the equilibrium morphology of the crystal grows into a developed side-branch structure, and the steady-state tip velocity of the facet dendrites increases linearly. The facet dendrite growth has controlled diffusion and kinetics.展开更多
Nine kinds of glass-ceramic matrix composites with different compositions and inter facial strength(L) were prepared. The influence of Ti on the fracture toughness (K1c.) of composites was studied. It was discoved tha...Nine kinds of glass-ceramic matrix composites with different compositions and inter facial strength(L) were prepared. The influence of Ti on the fracture toughness (K1c.) of composites was studied. It was discoved that, for the system no chemical reaction taking place at the interface, K1c. increased proportionallywith ts increasing at the first stage, then decreased when ts reached a certain value. According to this result,a model of relationship between L, thermal mismatch (Δαr) and K1c was built up. If a chemical reaction tookplace and a new phase was formed in the interface, the K1c. of composite was effected by the combination ofrs, chemical bonding, radial inter facial stress and other factors.展开更多
Protein folding involves the aminoacid sequence to come forth and form an energy minimized structure.Recently molecular crowding leading to increase in viscosity is said to be one of the major concerns affecting prote...Protein folding involves the aminoacid sequence to come forth and form an energy minimized structure.Recently molecular crowding leading to increase in viscosity is said to be one of the major concerns affecting protein folding.Many external fluorescent probes are used to detect such increases in viscosity.Since most of the protein sequences contain L-Phe and L-Trp,in this study we have used these aminoacids as probes to detect changes in viscosity.This study will help to advance the knowledge on molecular crowding effects in protein folding.展开更多
The shock-induced reaction mechanism and characteristics of Ni/Al system,considering an Al nanoparticle-embedded Ni single crystal,are investigated through molecular dynamics simulation.For the shock melting of Al nan...The shock-induced reaction mechanism and characteristics of Ni/Al system,considering an Al nanoparticle-embedded Ni single crystal,are investigated through molecular dynamics simulation.For the shock melting of Al nanoparticle,interfacial crystallization and dissolution are the main characteristics.The reaction degree of Al particle first increases linearly and then logarithmically with time driven by rapid mechanical mixing and following dissolution.The reaction rate increases with the decrease of particle diameter,however,the reaction is seriously hindered by interfacial crystallization when the diameter is lower than 9 nm in our simulations.Meanwhile,we found a negative exponential growth in the fraction of crystallized Al atoms,and the crystallinity of B2-NiAl(up to 20%)is positively correlated with the specific surface area of Al particle.This can be attributed to the formation mechanism of B2-NiAl by structural evolution of finite mixing layer near the collapsed interface.For shock melting of both Al particle and Ni matrix,the liquid-liquid phase inter-diffusion is the main reaction mechanism that can be enhanced by the formation of internal jet.In addition,the enhanced diffusion is manifested in the logarithmic growth law of mean square displacement,which results in an almost constant reaction rate similar to the mechanical mixing process.展开更多
Dispersion of ultrafine alumina suspension is examined by using particle size analyzer. The zeta potential and contact angle measurements were used to discuss the electrokinetic behavior and surface wettability of alu...Dispersion of ultrafine alumina suspension is examined by using particle size analyzer. The zeta potential and contact angle measurements were used to discuss the electrokinetic behavior and surface wettability of alumina in modifier solution, and to calculate the electrostatic interaction forces and interfacial interaction forces between alumina particles. The aggregation of ultrafine alumina occurs near its PZC. Addition of modifier increases the zeta potential of alumina and its surface hydrophilicity, resulting in increase of electrostatic and hydration repulsion. It makes the suspension of ultrafine alumina completely dispersed. The average particle size of the suspension is decreased from 1.73 μm in absence of modifier to 0.8 μm in the presence of tripolyphosphate. According to polar interfacial interaction approach, the hydration forces responsible for the stability of alumina suspension in the presence of modifier have also been obtained. The extended DLVO theory is successful to describe the dispersion behavior of ultrafine alumina in modifier solution.展开更多
Carbon fiber-reinforced carbon aerogel(C/CA)composites are one of the most promising candidates for applications requiring both thermal insulation and load bearing capabilities.The preparation of anti-oxidation coatin...Carbon fiber-reinforced carbon aerogel(C/CA)composites are one of the most promising candidates for applications requiring both thermal insulation and load bearing capabilities.The preparation of anti-oxidation coatings on C/CA to address its susceptibility to oxidation is a feasible approach to promote its application in oxidative environments.However,the currently reported coatings on C/CA mainly focus on improving the ablation performance and coating preparation process typically necessitating high-temperature heat treatment.This procedure can increase its thermal conductivity and reduce its thermal insulation ability.In this study,a series of ceramic-resin coatings were fabricated on C/CA through a simple slurry brushing-drying approach at room temperature.The effects of phenolic resin content on the coating structure,residual stress,thermal shock,and oxidation behaviors were investigated.Due to the adhesive properties and curing-induced shrinkage,the PR-7.5 coating(containing 7.5%(in mass)phenolic resin in the slurry)exhibits bonding strength close to fracture strength of the substrate and residual compressive stress of 0.853 GPa,which is beneficial for resisting thermal shock cracking.However,excessive resin content(PR-10.0 containing 10.0%(in mass)phenolic resin in the slurry)induces tensile stress due to uneven curing shrinkage,thereby leading to thermal shock cracking.Meanwhile,oxidation tests reveal significantly reduced weight losses for PR-7.5(17.46%at 800℃/100 min,8.15%at 1000℃/120 min,3.15%at 1200℃/120 min)versus uncoated C/CA’s 44.60%loss at 800℃/20 min.This work provides a brand-new and simple approach to improving the anti-oxidation performance of C/CA and expands its application in mild oxidative environments.展开更多
The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor ...The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.展开更多
UHMWPE(Ultra-High Molecular Weight Polyethylene)plain-weave fabric,characterized by its lightweight and high-strength properties,is widely used in protective equipment such as bulletproof vests and stab-resistant vest...UHMWPE(Ultra-High Molecular Weight Polyethylene)plain-weave fabric,characterized by its lightweight and high-strength properties,is widely used in protective equipment such as bulletproof vests and stab-resistant vests,serving as a key material for enhancing protective performance.This study systematically investigates the influence mechanism of interfacial properties on the energy absorption characteristics of UHMWPE-based protective structures through multi-scale experiments and numerical simulations,and establishes a cross-scale design methodology.Innovatively,an orthotropic constitutive model incorporating dynamic friction coefficients is constructed,combined with a modified Johnson-Cook failure criterion,to achieve high-precision simulation of the entire ballistic impact process(error<3.5%).Additionally,a friction field prediction model considering strain rate effects is developed,and the friction evolution laws of UHMWPE and Para-aramid(Kevlar)fabrics under strain rates of 10^(−3) and 10^(−4) s^(−1) are obtained through MTS pull-out tests.The results show that:(1)there exists a critical yarn-yarn friction coefficient(μ=0.2);exceeding this value leads to a 19%reduction in energy absorption capacity,while viscous interfaces increase the energy dissipation peak by 16%;(2)UHMWPE shows kinetically-dominated absorption(58%)with high rate but high load,increasing damage risk.Para-aramid has friction-dominated absorption(53%)with a lower rate but stable load.Hybrid fabrics use potential-dominated absorption(49%)at a moderate rate,balancing stability and protection.(3)3–5 layers of UHMWPE fabric yield optimal cost-effectiveness,with the unit cost reduction rate of the HS+5U scheme reaching 2.74 m/(s·$),which is 91%higher than that of the hybrid scheme.(4)For HS+5U(5-ply UHMWPE),V50 is 520 m/s,meeting primary protection requirement.For hybrid solutions with U/K≥3(e.g.,HS+6U+2K),V50 reaches 580 m/s(≥540 m/s),satisfying advanced protection requirement.This research provides critical references for the design of flexible protective structures and their engineering applications.展开更多
基金supported by the Initiative and Networking Fund of the Helmholtz Association(Grant No.VH-NG-1709)European Research Council(ERC)Starting Grant(MESO-CAT,Grant agreement No.101163405).
文摘Entropy is a basic thermodynamic property of the electrical double layer(EDL)at metal/solution interfaces,yet,its definition,measurement,and theoretical treatment are dispersed in the literature,and,in some cases,ambiguous.In this paper,we revisit the thermodynamic theory of EDL,from which two variants of entropy,excess entropy and formation entropy,are obtained and compared.In terms of the formation entropy,two calculation routes are validated in the context of a primitive EDL model,namely,the Gouy-Chapman(GC)model.After clarifying the concepts and calculation routes,we investigate interfacial water effects on the EDL entropy,using a refined Gouy-Chapman-Stern(GCS)model accounting for chemical potential difference between oxygen-and hydrogen-down water molecules,denotedδμ.The model-derived differential capacitance and entropy are compared with experimental data for the EDL at Au(111)in an aqueous electrolyte solution.The model reveals that the charge of maximum entropy(CME)is negative when water molecules have higher tendency to take oxygen-down configuration at the uncharged surface.Moreover,the formation entropy profile becomes asymmetric around the CME,whenδμis potential-dependent.However,the model fails to simultaneously reproduce capacitance and entropy measurements on the same system taken from two separate studies,indicating deficiencies of the model or experimental errors.Nevertheless,this work stresses the importance of measuring both capacitance and entropy of EDLs at the same time.
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.
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.
文摘The interfacial properties of steel-mushy Al-28Pb bonding plate with different interfacial structures, and the influence of ratio of Fe-Al compound at the interface on interfacial shear strength were investigated. The results show that there is a nonlinear relationship between the ratio of Fe-Al compound at the interface and the interfacial shear strength. When the ratio of Fe-Al compound at the interface is smaller than 71.4%, with the increase of the ratio of Fe-Al compound at the interface, the interfacial shear strength increases gradually; when the ratio of Fe-Al compound at the interface is larger than 71.4%, with the increase of the ratio of Fe-Al compound at the interface, the interfacial shear strength decreases continuously; when the ratio of Fe-Al compound at the interface is 71.4%, the largest interfacial shear strength 70.2MPa is obtained.
基金Projects(6512009004A,51908119,U1706222)supported by the National Natural Science Foundation of ChinaProject(BK20190367)supported by the Natural Science Foundation of Jiangsu Province,China。
文摘The interface properties between hydrated cement paste(hcp)and aggregates largely determine the various performances of concrete.In this work,molecular dynamics simulations were employed to explore the atomistic interaction mechanisms between the commonly used aggregate phase calcite/silica and calcium silicate hydrates(C-S-H),as well as the effect of moisture.The results suggest that the C-S-H/calcite interface is relatively strong and stable under both dry and moist conditions,which is caused by the high-strength interfacial connections formed between calcium ions from calcite and high-polarity non-bridging oxygen atoms from the C-S-H surface.Silica can be also adsorbed on the dry C-S-H surface by the H-bonds;however,the presence of water molecules on the interface may substantially decrease the affinities.Furthermore,the dynamics interface separation tests of C-S-H/aggregates were also implemented by molecular dynamics.The shape of the calculated stress-separation distance curves obeys the quasi-static cohesive law obtained experimentally.The moisture conditions and strain rates were found to affect the separation process of C-S-H/silica.A wetter interface and smaller loading rate may lead to a lower adhesion strength.The mechanisms interpreted here may shed new lights on the understandings of hcp/aggregate interactions at a nano-length scale and creation of high performance cementitious materials.
基金Project(2014BAB01B03)supported by the National Key Technology R&D Program During the 12th Five-Yean Plan of ChinaProject(51774286)supported by the National Natural Science Foundation of ChinaProject(BK20150192)supported by the Natural Science Foundation of Jiaaagsu Province,China
文摘The hydration film on particle surface plays an important role in bubble-particle adhesion in mineral flotation process. The thicknesses of the hydration films on natural hydrophobic coal and hydrophilic mica surfaces were measured directly by atomic force microscopy (AFM) based on the bending mode of the nominal constant compliance regime in AFM force curve in the present study. Surface and solid-liquid interfacial energies were calculated to explain the forming mechanism of the hydration film and atomic force microscopy data. The results show that there are significant differences in the structure and thickness of hydration films on coal and mica surfaces. Hydration film formed on mica surface with the thickness of 22.5 nm. In contrast, the bend was not detected in the nominal constant compliance regime. The van der Waals and polar interactions between both mica and coal and water molecules are characterized by an attractive effect, while the polar attractive free energy between water and mica (-87.36 mN/m) is significantly larger than that between water and coal (-32.89 mN/m), which leads to a thicker and firmer hydration layer on the mica surface. The interfacial interaction free energy of the coal/water/bubble is greater than that of mica. The polar attractive force is large enough to overcome the repulsive van der Waals force and the low energy barrier of film rupture, achieving coal particle bubble adhesion with a total interfacial free energy of-56.30 mN/m.
基金Projects(41977129,21607176,42007138) supported by the National Natural Science Foundation of ChinaProject(kq1802011) supported by the Changsha Outstanding Innovative Youth Training Program,ChinaProject(2017JJ3516)supported by the Natural Science Foundation of Hunan Province,China。
文摘A series of In_(x)Sb_(2-x)S_(3) nanosheets modified g-C_(3)N_(4)(In_(x)Sb_(2-x)S_(3)-TCN)heterojunctions with different g-C_(3)N_(4) contents were fabricated by an in situ deposition method.All the In_(x)Sb_(2-x)S_(3)-TCN composites were applied as photocatalysts in Cr(Ⅵ)polluted water treatment and the results displayed that In_(x)Sb_(2-x)S_(3)-TCN could effectively remove Cr(Ⅵ)under visible light through synergistic effects of adsorption and photocatalytic reduction.Especially,In_(x)Sb_(2-x)S_(3)-TCN-70(70 mg g-C_(3)N_(4)) exhibited the most excellent adsorption and photocatalytic reduction performance among all composites,which possessed a high equilibrium adsorption capacity of 12.45 mg/g in a 30.0 mg/L Cr(Ⅵ)aqueous solution,and reduced Cr(Ⅵ)to Cr(Ⅲ)within 10 min under visible light irradiation.DRS and PL results indicated that the interfacial coupling effect between g-C_(3)N_(4)and In_(x)Sb_(2-x)S_(3) enhanced the utilization efficiency of visible light and suppressed photoinduced carrier recombination,which improved the photocatalytic activity of composites.Moreover,the photocatalyst exhibited satisfactory reduction activity and good stability after 5 cycles of Cr(Ⅵ)adsorptionphotoreduction.
基金Project(50675234)supported by the National Natural Science Foundation of China
文摘Rapidly solidified Sn-9Zn-0.1Pr(/Nd) alloy foils were prepared by melt-spinning method. Through comparison, the effects of rapid solidification process and 0.1%Pr/Nd(mass fraction) addition on the microstructure, thermodynamic characteristic of Sn-9Zn solder alloy were analyzed. The tensile-shear tests were used to evaluate the mechanical properties of solder/Cu joints. The results show that the rapid solidification process can greatly refine the microstructure of Sn-9Zn-0.1Pr(/Nd) alloys. After rapid solidification, the effects of Pr/Nd addition on microstructure are depressed. The pasty range of the rapidly solidified Sn-Zn-RE solders is also reduced significantly. The mechanical properties of solder/Cu joints are obviously improved using the rapidly solidified Sn-9Zn-0.1Pr(/Nd) solder alloy, which results in the formation of uniform interface. The promotion effect of Nd addition in Sn-9Zn alloy on the interfacial reaction of solder/Cu joint is more remarkable than that of Pr.
基金the support for this work by National Natural Science Foundation of China(Grant Nos.22175139 and 22105156)。
文摘The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves the pretreatment of HMX to endow—OH groups on the surface via polyalcohol bonding agent modification and in situ coating with nitrate ester-containing polymer,was proposed to address the problem.Two types of energetic polyether—glycidyl azide polymer(GAP)and nitrate modified GAP(GNP)were grafted onto HMX crystal based on isocyanate addition reaction bridged through neutral polymeric bonding agent(NPBA)layer.The morphology and structure of the HMX-based composites were characterized in detail and the core-shell structure was validated.The grafted polymers obviously enhanced the adhesion force between HMX crystals and fluoropolymer(F2314)binder.Due to the interfacial reinforcement among the components,the two HMX-based composites exhibited a remarkable increment of phase transition peak temperature by 10.2°C and 19.6°C with no more than 1.5%shell content,respectively.Furthermore,the impact and friction sensitivity of the composites decreased significantly as a result of the barrier produced by the grafted polymers.These findings will enhance the future prospects for the interface design of energetic composites aiming to solve the weak interface and safety concerns.
基金Project (P1502) supported by Shanghai Leading Academic Discipline
文摘The organic phase separated from the interfacial crud provided by Dexing copper mine in Jiangxi, China, was analyzed by combined gas chromatography-mass spectroscopy. The results show that many kinds of emphiphiles containing such hydrophilic groups as carbonyl, carboxyl, sulphonyl or acylamine exist in organic phase. Conclusively, Lix984N would degrade gradually during a long-term contact with the acidic aqueous feed and strip reagents. Lix84 and nonylphenol as effective components of Lix984N degraded almost completely after long-term recycling. Lix984N degraded through such reactions as Beck.mann rearrange, hydrolysis and sulphofication. The degradation of Lix984N would deteriorate solvent extraction and disengagement performance, and result in a more stable interracial emulsion.
基金Project(2008AA03Z207) supported by the National Hi-tech Research and Development Program of China
文摘H+ doped polyaniline nanofibre(PH) was synthesized by interfacial polymerization and polyanilines doped with Li salt(PLI and PHLI) were prepared by immersing emeraldine base(EB) and H+ doped polyaniline in 1 mol/L LiPF6/(EC-EMC-DMC),respectively.PH,PLI and PHLI were all characterized by scanning electron microscopy(SEM) and Fourier transform infrared(FT-IR) spectrometry.With 1 mol/L LiPF6/(EC-EMC-DMC) as electrolyte,PH,PHLI and PLI were used as the active materials of symmetric non-aqueous redox supercapacitors.PLI shows the highest initial specific capacitance of 120 F/g(47 F/g for PH and 66 F/g for PHLI) among three samples.After 500 cycles,the specific capacitance of PLI remains 75 F/g,indicating the good cycleability.
基金Project(10834015) supported by the National Natural Science Foundation of ChinaProject(12SKY01-1) supported by the Doctoral Fund of Shangluo University,ChinaProject(14JK1223) supported by the Scientific Research Program of Shaanxi Provincial Education Department,China
文摘Numerical simulations based on a new regularized phase-field model were presented, to simulate the solidification of hexagonal close-packed materials with strong interfacial energy anisotropies. Results show that the crystal grows into facet dendrites,displaying six-fold symmetry. The size of initial crystals has an effect on the branching-off of the principal branch tip along the<100> direction, which is eliminated by setting the b/a(a and b are the semi-major and semi-minor sizes in the initial elliptical crystals, respectively) value to be less than or equal to 1. With an increase in the undercooling value, the equilibrium morphology of the crystal changes from a star-like shape to facet dendrites without side branches. The steady-state tip velocity increases exponentially when the dimensionless undercooling is below the critical value. With a further increase in the undercooling value, the equilibrium morphology of the crystal grows into a developed side-branch structure, and the steady-state tip velocity of the facet dendrites increases linearly. The facet dendrite growth has controlled diffusion and kinetics.
文摘Nine kinds of glass-ceramic matrix composites with different compositions and inter facial strength(L) were prepared. The influence of Ti on the fracture toughness (K1c.) of composites was studied. It was discoved that, for the system no chemical reaction taking place at the interface, K1c. increased proportionallywith ts increasing at the first stage, then decreased when ts reached a certain value. According to this result,a model of relationship between L, thermal mismatch (Δαr) and K1c was built up. If a chemical reaction tookplace and a new phase was formed in the interface, the K1c. of composite was effected by the combination ofrs, chemical bonding, radial inter facial stress and other factors.
文摘Protein folding involves the aminoacid sequence to come forth and form an energy minimized structure.Recently molecular crowding leading to increase in viscosity is said to be one of the major concerns affecting protein folding.Many external fluorescent probes are used to detect such increases in viscosity.Since most of the protein sequences contain L-Phe and L-Trp,in this study we have used these aminoacids as probes to detect changes in viscosity.This study will help to advance the knowledge on molecular crowding effects in protein folding.
基金supported by the State Key Program of National Natural Science Foundation of China(Grant No.12132003)State Key Laboratory of Explosion Science and Technology(Grant No.QNKT20-07)。
文摘The shock-induced reaction mechanism and characteristics of Ni/Al system,considering an Al nanoparticle-embedded Ni single crystal,are investigated through molecular dynamics simulation.For the shock melting of Al nanoparticle,interfacial crystallization and dissolution are the main characteristics.The reaction degree of Al particle first increases linearly and then logarithmically with time driven by rapid mechanical mixing and following dissolution.The reaction rate increases with the decrease of particle diameter,however,the reaction is seriously hindered by interfacial crystallization when the diameter is lower than 9 nm in our simulations.Meanwhile,we found a negative exponential growth in the fraction of crystallized Al atoms,and the crystallinity of B2-NiAl(up to 20%)is positively correlated with the specific surface area of Al particle.This can be attributed to the formation mechanism of B2-NiAl by structural evolution of finite mixing layer near the collapsed interface.For shock melting of both Al particle and Ni matrix,the liquid-liquid phase inter-diffusion is the main reaction mechanism that can be enhanced by the formation of internal jet.In addition,the enhanced diffusion is manifested in the logarithmic growth law of mean square displacement,which results in an almost constant reaction rate similar to the mechanical mixing process.
文摘Dispersion of ultrafine alumina suspension is examined by using particle size analyzer. The zeta potential and contact angle measurements were used to discuss the electrokinetic behavior and surface wettability of alumina in modifier solution, and to calculate the electrostatic interaction forces and interfacial interaction forces between alumina particles. The aggregation of ultrafine alumina occurs near its PZC. Addition of modifier increases the zeta potential of alumina and its surface hydrophilicity, resulting in increase of electrostatic and hydration repulsion. It makes the suspension of ultrafine alumina completely dispersed. The average particle size of the suspension is decreased from 1.73 μm in absence of modifier to 0.8 μm in the presence of tripolyphosphate. According to polar interfacial interaction approach, the hydration forces responsible for the stability of alumina suspension in the presence of modifier have also been obtained. The extended DLVO theory is successful to describe the dispersion behavior of ultrafine alumina in modifier solution.
基金National Natural Science Foundation of China(52272075,52472053)Research Fund of Youth Innovation Promotion Association of CAS,China(2021190)Defense Industrial Technology Development Program(JCKY2021130B007)。
文摘Carbon fiber-reinforced carbon aerogel(C/CA)composites are one of the most promising candidates for applications requiring both thermal insulation and load bearing capabilities.The preparation of anti-oxidation coatings on C/CA to address its susceptibility to oxidation is a feasible approach to promote its application in oxidative environments.However,the currently reported coatings on C/CA mainly focus on improving the ablation performance and coating preparation process typically necessitating high-temperature heat treatment.This procedure can increase its thermal conductivity and reduce its thermal insulation ability.In this study,a series of ceramic-resin coatings were fabricated on C/CA through a simple slurry brushing-drying approach at room temperature.The effects of phenolic resin content on the coating structure,residual stress,thermal shock,and oxidation behaviors were investigated.Due to the adhesive properties and curing-induced shrinkage,the PR-7.5 coating(containing 7.5%(in mass)phenolic resin in the slurry)exhibits bonding strength close to fracture strength of the substrate and residual compressive stress of 0.853 GPa,which is beneficial for resisting thermal shock cracking.However,excessive resin content(PR-10.0 containing 10.0%(in mass)phenolic resin in the slurry)induces tensile stress due to uneven curing shrinkage,thereby leading to thermal shock cracking.Meanwhile,oxidation tests reveal significantly reduced weight losses for PR-7.5(17.46%at 800℃/100 min,8.15%at 1000℃/120 min,3.15%at 1200℃/120 min)versus uncoated C/CA’s 44.60%loss at 800℃/20 min.This work provides a brand-new and simple approach to improving the anti-oxidation performance of C/CA and expands its application in mild oxidative environments.
文摘The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.
基金the Postdoctoral Science Foundation Funded Project of China with grant No.2021M701687Introduction and Education Plan for Young Innovative Talents in Colleges and Universities of Shandong Province.
文摘UHMWPE(Ultra-High Molecular Weight Polyethylene)plain-weave fabric,characterized by its lightweight and high-strength properties,is widely used in protective equipment such as bulletproof vests and stab-resistant vests,serving as a key material for enhancing protective performance.This study systematically investigates the influence mechanism of interfacial properties on the energy absorption characteristics of UHMWPE-based protective structures through multi-scale experiments and numerical simulations,and establishes a cross-scale design methodology.Innovatively,an orthotropic constitutive model incorporating dynamic friction coefficients is constructed,combined with a modified Johnson-Cook failure criterion,to achieve high-precision simulation of the entire ballistic impact process(error<3.5%).Additionally,a friction field prediction model considering strain rate effects is developed,and the friction evolution laws of UHMWPE and Para-aramid(Kevlar)fabrics under strain rates of 10^(−3) and 10^(−4) s^(−1) are obtained through MTS pull-out tests.The results show that:(1)there exists a critical yarn-yarn friction coefficient(μ=0.2);exceeding this value leads to a 19%reduction in energy absorption capacity,while viscous interfaces increase the energy dissipation peak by 16%;(2)UHMWPE shows kinetically-dominated absorption(58%)with high rate but high load,increasing damage risk.Para-aramid has friction-dominated absorption(53%)with a lower rate but stable load.Hybrid fabrics use potential-dominated absorption(49%)at a moderate rate,balancing stability and protection.(3)3–5 layers of UHMWPE fabric yield optimal cost-effectiveness,with the unit cost reduction rate of the HS+5U scheme reaching 2.74 m/(s·$),which is 91%higher than that of the hybrid scheme.(4)For HS+5U(5-ply UHMWPE),V50 is 520 m/s,meeting primary protection requirement.For hybrid solutions with U/K≥3(e.g.,HS+6U+2K),V50 reaches 580 m/s(≥540 m/s),satisfying advanced protection requirement.This research provides critical references for the design of flexible protective structures and their engineering applications.
