The interfacial interaction existing in the Ni ZrO 2 composite plating has been investigated. The experimental results show that no new phases were formed in the interfacial regions between matrix Ni and ZrO 2 part...The interfacial interaction existing in the Ni ZrO 2 composite plating has been investigated. The experimental results show that no new phases were formed in the interfacial regions between matrix Ni and ZrO 2 particles, but an orbital interaction through the mutual overlap of the d orbits does exist in the interfacial regions between Ni atoms and Zr 3+ ions.展开更多
A catalyst of ferroelectric-BaTiO_(3)@photoelectric-TiO_(2) nanohybrids(BaTiO_(3)@TiO_(2))with enhanced photocatalytic activity was synthesized via a hydrolysis precipitation combined with a hydrothermal approach.Comp...A catalyst of ferroelectric-BaTiO_(3)@photoelectric-TiO_(2) nanohybrids(BaTiO_(3)@TiO_(2))with enhanced photocatalytic activity was synthesized via a hydrolysis precipitation combined with a hydrothermal approach.Compared to pure TiO_(2),pure BaTiO_(3) and BaTiO_(3)/TiO_(2) physical mixture,the heterostructured BaTiO_(3)@TiO_(2) exhibits significantly improved photocatalytic activity and cycling stability in decomposing Rhodamine B(RhB)and the degradation efficiency is 1.7 times higher than pure TiO_(2) and 7.2 times higher than pure BaTiO_(3).These results are mainly attributed to the synergy effect of photoelectric TiO_(2),ferroelectric-BaTiO_(3) and the rationally designed interfacial structure.The mesoporous microstructure of TiO_(2) is of a high specific area and enables excellent photocatalytic activity.The ferroelectric polarization induced built-in electric field in BaTiO_(3) nanoparticles,and the intimate interfacial interactions at the interface of BaTiO_(3) and TiO_(2) are effective in driving the separation and transport of photogenerated charge carriers.This strategy will stimulate the design of heterostructured photocatalysts with outstanding photocatalytic performance via interface engineering.展开更多
Carbon catalysis is an attractive metal-free catalytic transformation,and its performance is significantly dependent on the number of accessible active sites.However,owing to the inherent stability of the C-C linkage,...Carbon catalysis is an attractive metal-free catalytic transformation,and its performance is significantly dependent on the number of accessible active sites.However,owing to the inherent stability of the C-C linkage,only limited active sites at the edge defects of the basal plane can be obtained even after a harsh oxidation treatment.In this study,the concept of interfacial interactions was adopted to propose an efficient strategy to develop highly active carbon catalysts.The alumina/carbon interface formed in situ acted as a cradle for the generation of oxygen-containing functional groups.In the absence of oxidation treatment,the concentration of oxygen-containing functional groups and the specific surface area can reach 1.27 mmol·g^(-1) and 2340 m^(2)·g^(-1),respectively,which are significantly higher than those of carbon prepared by traditional hard template methods.This active carbon shows a significant enhancement in catalytic performance in the oxidative coupling of amine to imine,about 22-fold higher than that of a well-known graphite oxide catalyst.Such interfacial interaction strategies are based on sustainable carbon sources and can effectively tune the porous structure of carbon in the micro-and meso-ranges.This conceptual finding offers new opportunities for the development of high-performance carbon-based metal-free catalysts.展开更多
The active sites of monodisperse transition metal Ni-clusters were anchored on carbon nitride(CN)by an in situ photoreduction deposition method to promote the efficient separation of photogenerated charges and achieve...The active sites of monodisperse transition metal Ni-clusters were anchored on carbon nitride(CN)by an in situ photoreduction deposition method to promote the efficient separation of photogenerated charges and achieve high-efficiency photocatalytic activity for hydrogen evolution.The Ni-cluster/CN exhibited a photocatalytic hydrogen production rate of 16.5 mmol·h^(-1)·g^(-1) and a total turnover frequency(TOF(H_(2)))value of 461.14 h^(-1).X-ray absorption spectroscopy based on synchrotron radiation indicated that CN had two reaction centers to form stable interface interactions with monodispersed Ni-clusters,in which carbon can act as an electron acceptor,while nitrogen can act as an electron donor.Meanwhile,the hybrid electronic structure of the Ni-cluster/CN system was constructed,which was favorable for photocatalytic activity for hydrogen production.An in-depth understanding of the interfacial interaction between CN and Ni-clusters will have important reference significance on the mechanistic study of development based on the cocatalyst.展开更多
Gold catalysts have been reported as highly effective catalysts in various oxidation reactions.However,for chemoselective hydrogenation reactions,gold‐based catalysts normally show much lowercatalytic activity than p...Gold catalysts have been reported as highly effective catalysts in various oxidation reactions.However,for chemoselective hydrogenation reactions,gold‐based catalysts normally show much lowercatalytic activity than platinum group metals,even though their selectivities are excellent.Here,wereport that the chemoselective hydrogenation activity of 3‐nitrostyrene to 3‐vinylaniline overAu/TiO_(2)can be enhanced up to 3.3 times through the hydrogen reduction strategy.It is revealedthat strong metal‐support interaction,between gold nanoparticles(NPs)and TiO_(2)support,is introducedthrough hydrogen reduction,resulting in partial dispersion of reduced TiOx on the Au surface.The partially covered Au not only increases the perimeter of the interface between the gold NPs andthe support,but also benefits H_(2)activation.Reaction kinetic analysis and H_(2)‐D2 exchange reactionshow that H_(2)activation is the critical step in the hydrogenation of 3‐nitrostyrene to 3‐vinylaniline.Density functional theory calculations verify that hydrogen dissociation and hydrogen transfer arefavored at the interface of gold NPs and TiO_(2)over the hydrogen‐reduced Au/TiO_(2).This study providesinsights for fabricating highly active gold‐based catalysts for chemoselective hydrogenationreactions.展开更多
The trajectory model of dispersed phase drops and distribution model of drop diameters were derived.By numerical simulation,the analytical results indicate that a large number of dispersed phase drops accumulate on th...The trajectory model of dispersed phase drops and distribution model of drop diameters were derived.By numerical simulation,the analytical results indicate that a large number of dispersed phase drops accumulate on the upper plate in different directions and form a hydrodynamic area with the stream-wise location in the range of 0—0.4m,where the flow of trickling film obtains kinetic drive from flowing field.The flowing field of trickling film exhibits an unstable state if the stream-wise location is less than 0.02m,and a stable state otherwise.Moreover,different velocity vectors of drops in the x-y plane result in different interactions between the trickling film and drops.For the non-uniform distribution of drop diameters,there is a stronger interaction between the trickling film and drop if the stream-wise location is less than 0.02m,because the amplitudes of velocity vectors are higher than those in the range of 0.02—1.0m.The result reveals a complexity and diversity of stratified two-phase flowing field.On the other hand,both the basic flowing field and distributions of drop diameters have a great influence on the distributions of comparable kinetic energy of drops.The complicated motions of larger drops are helpful to coalescence because they will consume much more kinetic energy on the trickling film than those of smaller drops.The change of comparable kinetic energy of smaller drops is continuous and steady.The smaller drops are easily entrained by the liquid-liquid flowing field.展开更多
Geogrid has been extensively used in geotechnical engineering practice due to its effectiveness and economy. Deep insight into the interaction between the backfill soil and the geogrid is of great importance for prope...Geogrid has been extensively used in geotechnical engineering practice due to its effectiveness and economy. Deep insight into the interaction between the backfill soil and the geogrid is of great importance for proper design and construction of geogrid reinforced earth structures. Based on the calibrated model of sand and geogrid, a series of numerical pullout tests are conducted using PFC^(3D) under special considerations of particle angularity and aperture geometry of the geogrid. In this work, interface characteristics regarding the displacement and contact force developed among particles and the deformation and force distribution along the geogrid are all visualized with PFC^(3D) simulations so that new understanding on how geogrid-soil interaction develops under pullout loads can be obtained. Meanwhile, a new variable named fabric anisotropy coefficient is introduced to evaluate the inherent relationship between macroscopic strength and microscopic fabric anisotropy. A correlation analysis is adopted to compare the accuracy between the newly-proposed coefficient and the most commonly used one. Furthermore, additional pullout tests on geogrid with four different joint protrusion heights have been conducted to investigate what extent and how vertical reinforcement elements may result in reinforcement effects from perspectives of bearing resistance contribution, energy dissipation, as well as volumetric response. Numerical results show that both the magnitude and the directional variation of normal contact forces govern the development of macroscopic strength and the reinforcing effects of joint protrusion height can be attributed to the accelerated energy dissipation across the particle assembly and the intensive mobilization of the geogrid.展开更多
The Kirchhoff thin elastic rod models are always the important basis to explore the configuration mecha- nism of the flexible structures in both the macroscopic and microscopic scale. As a continuum model of DNA, a th...The Kirchhoff thin elastic rod models are always the important basis to explore the configuration mecha- nism of the flexible structures in both the macroscopic and microscopic scale. As a continuum model of DNA, a thin elastic rod subjected to interfacial interactions is used to investigate the helical equilibrium configuration of DNA in salt solution. In this paper, the Kirchhoff's equations in the presence of interracial traction and the free energy density functions of different configurations are studied. The transition formula of the free energy between B-DNA and Z- DNA is obtained, and the results show that the free energy of the transition is mainly determined by the salt concentra- tion, which agrees well with the experimental data.展开更多
Abstract: In this work, the authors present a study of growth and characterization of composite based on AI and CNT (carbon nanotubes. The composites were prepared by a chemical mixing method and characterized by SE...Abstract: In this work, the authors present a study of growth and characterization of composite based on AI and CNT (carbon nanotubes. The composites were prepared by a chemical mixing method and characterized by SEM analysis, energy dispersed X-ray measurements, X-ray photoelectron spectroscopy and cathodoluminescence spectroscopy. The analysis showed that the composites are formed by macro-cluster of aluminum oxide on a network of CNT without formation of chemical bonds at interface between particles. The results are compared with those obtained for a sample of CNT with AI traces (〈 0.5%). They show that only the presence of metal traces changes the nanotubes optical properties, with a luminescence signal centered at about 380 nm. These luminescence signals are caused by the adhesion between CNT and AI micro-clusters that promote the formation of band gap with some local energy levels.展开更多
This paper describes the research carried out in partial fulfilment of the degree of doctor of education. The study was qualitative in nature with a phenomenological interpretive paradigm dominating the philosophical ...This paper describes the research carried out in partial fulfilment of the degree of doctor of education. The study was qualitative in nature with a phenomenological interpretive paradigm dominating the philosophical approach. The research methods adopted combined life story and grounded theory. As far as the author has been able to determine there are very few, if any studies which have applied this approach specifically to this area of research which investigated the influence life history has on attitude to lifelong learning. Twenty five respondents were interviewed in face-to-face informal interviews. The main aim was to elicit the respondent's subjective interpretation of the interaction between school, family, work, and learning within their lives. The researcher was then able to identify when they occurred and what or who made them particularly meaningful. This paper describes how initial decisions were made regarding the substantive area for the research. Sampling technique and method for collecting the data is discussed and a worked example is given of how the data was analysed. It is intended that this paper will give an insight into the challenge of combining these two much debated methods of research. The empirical data lead to some interesting findings which educators and policy makers will find helpful in order to strengthen the school, college, and workplace interface.展开更多
Typical cationic and anionic surfactants were chosen and their interactions were calculated by quantum chemical method. Interaction energies are -0.2378 kJ·mol-1, -3.3394kJ·mol-1 and 0.1204kJ·mol-1 for ...Typical cationic and anionic surfactants were chosen and their interactions were calculated by quantum chemical method. Interaction energies are -0.2378 kJ·mol-1, -3.3394kJ·mol-1 and 0.1204kJ·mol-1 for the molecular pairs with fluocarbon and hydrocarbon chain: C4H10/C5H12, C4F10/C5H12, and C4F10 /C5F12, respectively. When hydrophilic group with cationic and anionicions is introduced, interaction energies are -287.40kJ·mol-1, -311.18kJ·mol-1 and -345.83kJ·mol-1. The results show that there is strong static interaction between cationic and anionic surfactants. It has been predicted that mixed monolayer may be formed and surface activity is enhanced favorably, especially for mixtures of cationic and anionic surfactants with fluocarbon and hydrocarbon chains. The anionic surfactants, sodium octadecylbenzenesulfonate perfluopolyetherbenzenesulonate(ANF-I) was synthesized, mixture effects of ANF-I with sodium octadecylbenzenesulfonate or dodecyldimethyl benzylammonium bromide were studied. The results indicate that the efficiency of mixing increased and the theoretical prediction was testified. These results can provide useful information for the design of new surfactants.展开更多
Solid-aqueous interfaces and phenomena occurring at those interfaces are ubiquitously found in a plethora of chemical systems.When it comes to heterogeneous catalysis,however,our understanding of chemical transformati...Solid-aqueous interfaces and phenomena occurring at those interfaces are ubiquitously found in a plethora of chemical systems.When it comes to heterogeneous catalysis,however,our understanding of chemical transformations at solid-aqueous interfaces is relatively limited and primitive.This review phenomenologically describes a selection of water-engendered effects on the catalytic behavior for several prototypical acid-base-catalyzed reactions over solid catalysts,and critically assesses the general and special roles of water molecules,structural moieties derived from water,and ionic species that are dissolved in it,with an aim to extract novel concepts and principles that underpin heterogeneous acid-base catalysis in the aqueous phase.For alcohol dehydration catalyzed by solid Bronsted acids,rate inhibition by water is most typically related to the decrease in the acid strength and/or the preferential solvation of adsorbed species over the transition state as water molecules progressively solvate the acid site and form extended networks wherein protons are mobilized.Water also inhibits dehydration kinetics over most Lewis acid-base catalysts by competitive adsorption,but a few scattered reports reveal substantial rate enhancements due to the conversion of Lewis acid sites to Brønsted acid sites with higher catalytic activities upon the introduction of water.For aldol condensation on catalysts exposing Lewis acid-base pairs,the addition of water is generally observed to enhance the rate when C–C coupling is rate-limiting,but may result in rate inhibition by site-blocking when the initial unimolecular deprotonation is rate-limiting.Water can also promote aldol condensation on Brønsted acidic catalysts by facilitating inter-site communication between acid sites through hydrogen-bonding interactions.For metallozeolite-catalyzed sugar isomerization in aqueous media,the nucleation and networking of intrapore waters regulated by hydrophilic entities causes characteristic enthalpy-entropy tradeoffs as these water moieties interact with kinetically relevant hydride transfer transition states.The discussed examples collectively highlight the utmost importance of hydrogen-bonding interactions and ionization of covalently bonded surface moieties as the main factors underlying the uniqueness of water-mediated interfacial acid-base chemistries and the associated solvation effects in the aqueous phase or in the presence of water.A perspective is also provided for future research in this vibrant field.展开更多
The communication reports an exploratory experimental study on the effects of nitrogen annealing on lithium ion intercalation in nickel-doped lithium trivana- date cathodic electrodes for lithium ion batteries. It sho...The communication reports an exploratory experimental study on the effects of nitrogen annealing on lithium ion intercalation in nickel-doped lithium trivana- date cathodic electrodes for lithium ion batteries. It shows good rate performance with discharge capacities of 348.6, 252.6, 191.9 and 96.7 mAh g-1 at 0.2, 0.5, 1 and 5 C, respectively. Nitrogen annealing resulted in the formation of parasitic secondary-phase LiVzO5 and appreciably increased tetravalent vanadium ions compensated with oxygen vacancies, which would enhance the electronic conductivity and lithium ion diffusivity and promote the interface interaction and deintercalation process, and thus lead to the enhanced lithium ion intercalation properties. The possible impacts of the parasitic secondary-phase LiV205 on the lithium ion intercalation performance have also been discussed.展开更多
The morphology of sediment particles plays an important role in interfacial interactions.The difficulties in complex morphological description significantly limit the research on interfacial interactions.In this study...The morphology of sediment particles plays an important role in interfacial interactions.The difficulties in complex morphological description significantly limit the research on interfacial interactions.In this study,images of a single sediment particle extracted from electron microscope photos were used to analyze the gray values and present the probability of shape of the sediment particles.Moreover,the morphological features of the sediment particles were qualitatively described using the fractal method(surface area-volume method).The fractal dimension D of a single sediment particle was calculated to analyze the features and quantitative complexity of the sediment particle morphology.Results indicate that the probability of shape can provide intuitive morphological structure and fully describe the complex morphological characteristics of sediment particle surfaces.The fractal dimension abstractly described the complexity of the morphology of a sediment particle surface and matched well with the experimental results.The methods discussed in this study are suitable for describing the complex morphology of the sediment particle surface and lay the scientific foundation for further research on the interfacial interaction between the sediment particle and the pollutant.展开更多
Alloyed nanoparticles with core-shell structures provide a favorable model to modulate interfacial interaction and surface structures at the atomic level,which is important for designing electrocatalysts with high act...Alloyed nanoparticles with core-shell structures provide a favorable model to modulate interfacial interaction and surface structures at the atomic level,which is important for designing electrocatalysts with high activity and durability.Herein,core-shell structured Pd3M@Pt/C nanoparticles with binary PdM alloy cores(M=Fe,Ni,and Co)and a monolayer Pt shell were successfully synthesized with diverse interfaces.Among these,Pd3Fe@Pt/C exhibited the best oxygen reduction reaction catalytic performance,roughly 5.4 times more than that of the commercial Pt/C catalyst used as reference.The significantly enhanced activity is attributed to the combined effects of strain engineering,interfacial electron transfer,and improved Pt utilization.Density functional theory simulations and extended X-ray absorption fine structure analysis revealed that engineering the alloy core with moderate lattice mismatch and alloy composition(Pd3Fe)optimizes the surface oxygen adsorption energy,thereby rendering excellent electrocatalytic activity.Future researches may use this study as a guide on the construction of highly effective core-shell electrocatalysts for various energy conversions and other applications.展开更多
The hierarchical micro/nanoscale layered formation of organic and inorganic components of natural nacre, results in abundant interracial interactions, providing an inspiration for fabricating bioinspired nanocomposite...The hierarchical micro/nanoscale layered formation of organic and inorganic components of natural nacre, results in abundant interracial interactions, providing an inspiration for fabricating bioinspired nanocomposites through constructing the interfacial interactions. Herein, we demonstrated the synergistic interfacial interactions of hydrogen bonding from hydroxypropyl cellu- lose and ionic bonding from copper ions upon the reduced graphene oxide based bioinspired nanocomposites, which show the integrated tensile strength, toughness and excellent fatigue-resistant property, as well as high electrical conductivity. These ex- traordinary properties allow this kind of bioinspired nanocomposites to potentially utilize in the fields of aerospace, flexible electronics devices, etc. This study also opens a door for fabricating excellent mechanical performance graphene-based bioin- spired nanocomposites via synergistic interfacial interactions in the future.展开更多
Nonprecious metal-based oxygen reduction reaction(ORR)electrocatalysts with high efficiency in both alkaline and acidic media are being intensively studied for the purpose of replacing expensive Pt-based catalysts;how...Nonprecious metal-based oxygen reduction reaction(ORR)electrocatalysts with high efficiency in both alkaline and acidic media are being intensively studied for the purpose of replacing expensive Pt-based catalysts;however,it is still a challenge to achieve superior ORR performances,especially in acidic media.Herein,by pyrolysis of mixed precursors of diammonium phosphate,melamine and hemin,we prepared a nanocomposite catalyst(denoted as FeP@PGL)composed of nitrogen-doped carbon nanosheets with embedded FeP nanoparticles(NPs),which were encapsulated by in-situ formed phosphorus-doped graphene layers.It is found that phosphorous was preferentially doped in the coating layers on FeP NPs,instead of in the carbon nanosheets.The FeP@PGL catalyst exhibited excellent ORR performance,with the onset and half-wave potential up to 1.01 and 0.90 V vs.the reversible hydrogen electrode(RHE)in alkaline media,and0.95 and 0.81 V vs.RHE in acidic media,respectively.By thorough microscopy and spectroscopy characterizations,the interfacial charge transfer between the encapsulated FeP NPs and P-doped graphene layers was identified,and the local work function of the catalyst surface was also reduced by the interfacial interaction.The interfacial synergy between the encapsulated FeP and phosphorus-doped graphene layers was essential to enhance the ORR performance.This study not only demonstrates the promising ORR properties of the encapsulated-FeP-based nanocomposite catalyst,but also provides direct evidence of the interfacial charge transfer effect and its role in ORR process.展开更多
Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction(HOR) and hydrogen evolution reaction(HER) due to its similar binding energy towards *H but lower price compared to Pt.Nevertheless,...Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction(HOR) and hydrogen evolution reaction(HER) due to its similar binding energy towards *H but lower price compared to Pt.Nevertheless, the quest of high-efficiency Ru-based catalysts for HOR and HER is driven by the current disadvantages including low activity and unsatisfactory stability. Herein, we have fabricated and engineered two-dimensional(2D) Ru-based snow-like nanosheets with Ru/Ru O2interface(Ru/Ru O2SNSs)via a post-annealing treatment. Detailed characterizations and theoretical calculations indicate that the interfacial synergy, which is dependent on the temperature for annealing, can alter the hydrogen binding energy(HBE) and hydroxide binding energy(OHBE), as a result of the enhanced HOR and HER performance. Impressively, the optimal Ru/RuO_(2) SNSs display a mass activity of 9.13 A mgRu^(–1) at an overpotential of 50 m V in 0.1 mol L^(–1) KOH for HOR, which is 65, 304, and 21 times higher than those of Ru SNSs(0.14 A mg_(Ru)^(–1)), RuO_(2) SNSs(0.03 A mg_(Ru)^(–1)), and commercial Pt/C(0.43 A mg_(Ru)^(–1)), respectively.Moreover, Ru/RuO_(2) SNSs display improved HER activity with a low overpotential of 20.2 m V for achieving10 m A cm^(-2)in 1 mol L^(–1)KOH. This work not only provides an efficient catalyst for HOR and HER, but also promotes fundamental research on the fabrication and modification of catalysts in heterogeneous catalysis.展开更多
文摘The interfacial interaction existing in the Ni ZrO 2 composite plating has been investigated. The experimental results show that no new phases were formed in the interfacial regions between matrix Ni and ZrO 2 particles, but an orbital interaction through the mutual overlap of the d orbits does exist in the interfacial regions between Ni atoms and Zr 3+ ions.
基金Project(cstc2020jcyj-msxm X0930) supported by the Natural Science Foundation of Chongqing,ChinaProject(KJQN201901522) supported by Technological Research Program of Chongqing Municipal Education Commission,ChinaProject(cx2020068) supported by the Venture&Innovation Support Program for Chongqing Overseas Returnees,China。
文摘A catalyst of ferroelectric-BaTiO_(3)@photoelectric-TiO_(2) nanohybrids(BaTiO_(3)@TiO_(2))with enhanced photocatalytic activity was synthesized via a hydrolysis precipitation combined with a hydrothermal approach.Compared to pure TiO_(2),pure BaTiO_(3) and BaTiO_(3)/TiO_(2) physical mixture,the heterostructured BaTiO_(3)@TiO_(2) exhibits significantly improved photocatalytic activity and cycling stability in decomposing Rhodamine B(RhB)and the degradation efficiency is 1.7 times higher than pure TiO_(2) and 7.2 times higher than pure BaTiO_(3).These results are mainly attributed to the synergy effect of photoelectric TiO_(2),ferroelectric-BaTiO_(3) and the rationally designed interfacial structure.The mesoporous microstructure of TiO_(2) is of a high specific area and enables excellent photocatalytic activity.The ferroelectric polarization induced built-in electric field in BaTiO_(3) nanoparticles,and the intimate interfacial interactions at the interface of BaTiO_(3) and TiO_(2) are effective in driving the separation and transport of photogenerated charge carriers.This strategy will stimulate the design of heterostructured photocatalysts with outstanding photocatalytic performance via interface engineering.
文摘Carbon catalysis is an attractive metal-free catalytic transformation,and its performance is significantly dependent on the number of accessible active sites.However,owing to the inherent stability of the C-C linkage,only limited active sites at the edge defects of the basal plane can be obtained even after a harsh oxidation treatment.In this study,the concept of interfacial interactions was adopted to propose an efficient strategy to develop highly active carbon catalysts.The alumina/carbon interface formed in situ acted as a cradle for the generation of oxygen-containing functional groups.In the absence of oxidation treatment,the concentration of oxygen-containing functional groups and the specific surface area can reach 1.27 mmol·g^(-1) and 2340 m^(2)·g^(-1),respectively,which are significantly higher than those of carbon prepared by traditional hard template methods.This active carbon shows a significant enhancement in catalytic performance in the oxidative coupling of amine to imine,about 22-fold higher than that of a well-known graphite oxide catalyst.Such interfacial interaction strategies are based on sustainable carbon sources and can effectively tune the porous structure of carbon in the micro-and meso-ranges.This conceptual finding offers new opportunities for the development of high-performance carbon-based metal-free catalysts.
文摘The active sites of monodisperse transition metal Ni-clusters were anchored on carbon nitride(CN)by an in situ photoreduction deposition method to promote the efficient separation of photogenerated charges and achieve high-efficiency photocatalytic activity for hydrogen evolution.The Ni-cluster/CN exhibited a photocatalytic hydrogen production rate of 16.5 mmol·h^(-1)·g^(-1) and a total turnover frequency(TOF(H_(2)))value of 461.14 h^(-1).X-ray absorption spectroscopy based on synchrotron radiation indicated that CN had two reaction centers to form stable interface interactions with monodispersed Ni-clusters,in which carbon can act as an electron acceptor,while nitrogen can act as an electron donor.Meanwhile,the hybrid electronic structure of the Ni-cluster/CN system was constructed,which was favorable for photocatalytic activity for hydrogen production.An in-depth understanding of the interfacial interaction between CN and Ni-clusters will have important reference significance on the mechanistic study of development based on the cocatalyst.
文摘Gold catalysts have been reported as highly effective catalysts in various oxidation reactions.However,for chemoselective hydrogenation reactions,gold‐based catalysts normally show much lowercatalytic activity than platinum group metals,even though their selectivities are excellent.Here,wereport that the chemoselective hydrogenation activity of 3‐nitrostyrene to 3‐vinylaniline overAu/TiO_(2)can be enhanced up to 3.3 times through the hydrogen reduction strategy.It is revealedthat strong metal‐support interaction,between gold nanoparticles(NPs)and TiO_(2)support,is introducedthrough hydrogen reduction,resulting in partial dispersion of reduced TiOx on the Au surface.The partially covered Au not only increases the perimeter of the interface between the gold NPs andthe support,but also benefits H_(2)activation.Reaction kinetic analysis and H_(2)‐D2 exchange reactionshow that H_(2)activation is the critical step in the hydrogenation of 3‐nitrostyrene to 3‐vinylaniline.Density functional theory calculations verify that hydrogen dissociation and hydrogen transfer arefavored at the interface of gold NPs and TiO_(2)over the hydrogen‐reduced Au/TiO_(2).This study providesinsights for fabricating highly active gold‐based catalysts for chemoselective hydrogenationreactions.
基金Supported by Natural Science Foundation of Tianjin (No.09JCYBJC06400,No.10 JCZDJC23300)
文摘The trajectory model of dispersed phase drops and distribution model of drop diameters were derived.By numerical simulation,the analytical results indicate that a large number of dispersed phase drops accumulate on the upper plate in different directions and form a hydrodynamic area with the stream-wise location in the range of 0—0.4m,where the flow of trickling film obtains kinetic drive from flowing field.The flowing field of trickling film exhibits an unstable state if the stream-wise location is less than 0.02m,and a stable state otherwise.Moreover,different velocity vectors of drops in the x-y plane result in different interactions between the trickling film and drops.For the non-uniform distribution of drop diameters,there is a stronger interaction between the trickling film and drop if the stream-wise location is less than 0.02m,because the amplitudes of velocity vectors are higher than those in the range of 0.02—1.0m.The result reveals a complexity and diversity of stratified two-phase flowing field.On the other hand,both the basic flowing field and distributions of drop diameters have a great influence on the distributions of comparable kinetic energy of drops.The complicated motions of larger drops are helpful to coalescence because they will consume much more kinetic energy on the trickling film than those of smaller drops.The change of comparable kinetic energy of smaller drops is continuous and steady.The smaller drops are easily entrained by the liquid-liquid flowing field.
基金Projects(51278216,51478201)supported by the National Natural Science Foundation of China
文摘Geogrid has been extensively used in geotechnical engineering practice due to its effectiveness and economy. Deep insight into the interaction between the backfill soil and the geogrid is of great importance for proper design and construction of geogrid reinforced earth structures. Based on the calibrated model of sand and geogrid, a series of numerical pullout tests are conducted using PFC^(3D) under special considerations of particle angularity and aperture geometry of the geogrid. In this work, interface characteristics regarding the displacement and contact force developed among particles and the deformation and force distribution along the geogrid are all visualized with PFC^(3D) simulations so that new understanding on how geogrid-soil interaction develops under pullout loads can be obtained. Meanwhile, a new variable named fabric anisotropy coefficient is introduced to evaluate the inherent relationship between macroscopic strength and microscopic fabric anisotropy. A correlation analysis is adopted to compare the accuracy between the newly-proposed coefficient and the most commonly used one. Furthermore, additional pullout tests on geogrid with four different joint protrusion heights have been conducted to investigate what extent and how vertical reinforcement elements may result in reinforcement effects from perspectives of bearing resistance contribution, energy dissipation, as well as volumetric response. Numerical results show that both the magnitude and the directional variation of normal contact forces govern the development of macroscopic strength and the reinforcing effects of joint protrusion height can be attributed to the accelerated energy dissipation across the particle assembly and the intensive mobilization of the geogrid.
基金Supported by the National Nature Science Foundation of China(No.11372210)the Research Fund for the Doctoral Program of Higher Education of China(No.20120032110010)Tianjin Research Program of Application Foundation and Advanced Technology(No.12JCZDJC28000)
文摘The Kirchhoff thin elastic rod models are always the important basis to explore the configuration mecha- nism of the flexible structures in both the macroscopic and microscopic scale. As a continuum model of DNA, a thin elastic rod subjected to interfacial interactions is used to investigate the helical equilibrium configuration of DNA in salt solution. In this paper, the Kirchhoff's equations in the presence of interracial traction and the free energy density functions of different configurations are studied. The transition formula of the free energy between B-DNA and Z- DNA is obtained, and the results show that the free energy of the transition is mainly determined by the salt concentra- tion, which agrees well with the experimental data.
文摘Abstract: In this work, the authors present a study of growth and characterization of composite based on AI and CNT (carbon nanotubes. The composites were prepared by a chemical mixing method and characterized by SEM analysis, energy dispersed X-ray measurements, X-ray photoelectron spectroscopy and cathodoluminescence spectroscopy. The analysis showed that the composites are formed by macro-cluster of aluminum oxide on a network of CNT without formation of chemical bonds at interface between particles. The results are compared with those obtained for a sample of CNT with AI traces (〈 0.5%). They show that only the presence of metal traces changes the nanotubes optical properties, with a luminescence signal centered at about 380 nm. These luminescence signals are caused by the adhesion between CNT and AI micro-clusters that promote the formation of band gap with some local energy levels.
文摘This paper describes the research carried out in partial fulfilment of the degree of doctor of education. The study was qualitative in nature with a phenomenological interpretive paradigm dominating the philosophical approach. The research methods adopted combined life story and grounded theory. As far as the author has been able to determine there are very few, if any studies which have applied this approach specifically to this area of research which investigated the influence life history has on attitude to lifelong learning. Twenty five respondents were interviewed in face-to-face informal interviews. The main aim was to elicit the respondent's subjective interpretation of the interaction between school, family, work, and learning within their lives. The researcher was then able to identify when they occurred and what or who made them particularly meaningful. This paper describes how initial decisions were made regarding the substantive area for the research. Sampling technique and method for collecting the data is discussed and a worked example is given of how the data was analysed. It is intended that this paper will give an insight into the challenge of combining these two much debated methods of research. The empirical data lead to some interesting findings which educators and policy makers will find helpful in order to strengthen the school, college, and workplace interface.
文摘Typical cationic and anionic surfactants were chosen and their interactions were calculated by quantum chemical method. Interaction energies are -0.2378 kJ·mol-1, -3.3394kJ·mol-1 and 0.1204kJ·mol-1 for the molecular pairs with fluocarbon and hydrocarbon chain: C4H10/C5H12, C4F10/C5H12, and C4F10 /C5F12, respectively. When hydrophilic group with cationic and anionicions is introduced, interaction energies are -287.40kJ·mol-1, -311.18kJ·mol-1 and -345.83kJ·mol-1. The results show that there is strong static interaction between cationic and anionic surfactants. It has been predicted that mixed monolayer may be formed and surface activity is enhanced favorably, especially for mixtures of cationic and anionic surfactants with fluocarbon and hydrocarbon chains. The anionic surfactants, sodium octadecylbenzenesulfonate perfluopolyetherbenzenesulonate(ANF-I) was synthesized, mixture effects of ANF-I with sodium octadecylbenzenesulfonate or dodecyldimethyl benzylammonium bromide were studied. The results indicate that the efficiency of mixing increased and the theoretical prediction was testified. These results can provide useful information for the design of new surfactants.
文摘Solid-aqueous interfaces and phenomena occurring at those interfaces are ubiquitously found in a plethora of chemical systems.When it comes to heterogeneous catalysis,however,our understanding of chemical transformations at solid-aqueous interfaces is relatively limited and primitive.This review phenomenologically describes a selection of water-engendered effects on the catalytic behavior for several prototypical acid-base-catalyzed reactions over solid catalysts,and critically assesses the general and special roles of water molecules,structural moieties derived from water,and ionic species that are dissolved in it,with an aim to extract novel concepts and principles that underpin heterogeneous acid-base catalysis in the aqueous phase.For alcohol dehydration catalyzed by solid Bronsted acids,rate inhibition by water is most typically related to the decrease in the acid strength and/or the preferential solvation of adsorbed species over the transition state as water molecules progressively solvate the acid site and form extended networks wherein protons are mobilized.Water also inhibits dehydration kinetics over most Lewis acid-base catalysts by competitive adsorption,but a few scattered reports reveal substantial rate enhancements due to the conversion of Lewis acid sites to Brønsted acid sites with higher catalytic activities upon the introduction of water.For aldol condensation on catalysts exposing Lewis acid-base pairs,the addition of water is generally observed to enhance the rate when C–C coupling is rate-limiting,but may result in rate inhibition by site-blocking when the initial unimolecular deprotonation is rate-limiting.Water can also promote aldol condensation on Brønsted acidic catalysts by facilitating inter-site communication between acid sites through hydrogen-bonding interactions.For metallozeolite-catalyzed sugar isomerization in aqueous media,the nucleation and networking of intrapore waters regulated by hydrophilic entities causes characteristic enthalpy-entropy tradeoffs as these water moieties interact with kinetically relevant hydride transfer transition states.The discussed examples collectively highlight the utmost importance of hydrogen-bonding interactions and ionization of covalently bonded surface moieties as the main factors underlying the uniqueness of water-mediated interfacial acid-base chemistries and the associated solvation effects in the aqueous phase or in the presence of water.A perspective is also provided for future research in this vibrant field.
基金supported by the‘‘Thousands Talents’’Program for a pioneer researcher and his innovative teamChina+5 种基金supported by the National Natural Science Foundation of China(51374029)the National Science Foundation(NSFDMR-1505902)Program for New Century Excellent Talents in University(NCET-13-0668)Fundamental Research Funds for the Central Universities(FRF-TP-14-008C1)China Postdoctoral Science Foundation(2015M570988)
文摘The communication reports an exploratory experimental study on the effects of nitrogen annealing on lithium ion intercalation in nickel-doped lithium trivana- date cathodic electrodes for lithium ion batteries. It shows good rate performance with discharge capacities of 348.6, 252.6, 191.9 and 96.7 mAh g-1 at 0.2, 0.5, 1 and 5 C, respectively. Nitrogen annealing resulted in the formation of parasitic secondary-phase LiVzO5 and appreciably increased tetravalent vanadium ions compensated with oxygen vacancies, which would enhance the electronic conductivity and lithium ion diffusivity and promote the interface interaction and deintercalation process, and thus lead to the enhanced lithium ion intercalation properties. The possible impacts of the parasitic secondary-phase LiV205 on the lithium ion intercalation performance have also been discussed.
基金supported by the National Natural Science Foundation of China (Grant No. 50909107)the China Post-doctoral Science Special Foundation (Grant No. 201003385)Young Teachers Cultivation Project from Sun Yat-sen University (Grant No. 37000-3161402)
文摘The morphology of sediment particles plays an important role in interfacial interactions.The difficulties in complex morphological description significantly limit the research on interfacial interactions.In this study,images of a single sediment particle extracted from electron microscope photos were used to analyze the gray values and present the probability of shape of the sediment particles.Moreover,the morphological features of the sediment particles were qualitatively described using the fractal method(surface area-volume method).The fractal dimension D of a single sediment particle was calculated to analyze the features and quantitative complexity of the sediment particle morphology.Results indicate that the probability of shape can provide intuitive morphological structure and fully describe the complex morphological characteristics of sediment particle surfaces.The fractal dimension abstractly described the complexity of the morphology of a sediment particle surface and matched well with the experimental results.The methods discussed in this study are suitable for describing the complex morphology of the sediment particle surface and lay the scientific foundation for further research on the interfacial interaction between the sediment particle and the pollutant.
基金the Natural Science Foundation of Hainan Province(2019RC007)the National Natural Science Foundation of China(21805104,21606050,21905056,21905045,and U1801257)+3 种基金the Natural Science Foundation of Guangdong Province(2018A0303130239,2018A0303130223)Pearl River Science and Technology New Star Project(201806010039)the Start-up Research Foundation of Hainan University(KYQD(ZR)1908)Research Fund Program of Key Laboratory of Fuel Cell Technology of Guangdong Province。
文摘Alloyed nanoparticles with core-shell structures provide a favorable model to modulate interfacial interaction and surface structures at the atomic level,which is important for designing electrocatalysts with high activity and durability.Herein,core-shell structured Pd3M@Pt/C nanoparticles with binary PdM alloy cores(M=Fe,Ni,and Co)and a monolayer Pt shell were successfully synthesized with diverse interfaces.Among these,Pd3Fe@Pt/C exhibited the best oxygen reduction reaction catalytic performance,roughly 5.4 times more than that of the commercial Pt/C catalyst used as reference.The significantly enhanced activity is attributed to the combined effects of strain engineering,interfacial electron transfer,and improved Pt utilization.Density functional theory simulations and extended X-ray absorption fine structure analysis revealed that engineering the alloy core with moderate lattice mismatch and alloy composition(Pd3Fe)optimizes the surface oxygen adsorption energy,thereby rendering excellent electrocatalytic activity.Future researches may use this study as a guide on the construction of highly effective core-shell electrocatalysts for various energy conversions and other applications.
基金supported by the Excellent Young Scientist Foundation of NSFC(Grant No.51522301)the National Natural Science Foundation of China(Grant Nos.21273017&51103004)+7 种基金Program for New Century Excellent Talents in University(Grant No.NCET-12-0034)Beijing Nova Program(Grant No.Z121103002512020)Fok Ying-Tong Education Foundation(Grant No.141045)Open Project of Beijing National Laboratory for Molecular Sciences,the 111 Project(Grant No.B14009)Aeronautical Science Foundation of China(Grant Nos.20145251035&2015ZF21009)State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,Donghua University(Grant No.LK1508)the Key Research Program of the Chinese Academy of Sciences(Grant No.KJZD-EW-M03)the Fundamental Research Funds for the Central Universities(Grant Nos.YWF-15-HHXY-001&YWF-16-BJ-J-09)
文摘The hierarchical micro/nanoscale layered formation of organic and inorganic components of natural nacre, results in abundant interracial interactions, providing an inspiration for fabricating bioinspired nanocomposites through constructing the interfacial interactions. Herein, we demonstrated the synergistic interfacial interactions of hydrogen bonding from hydroxypropyl cellu- lose and ionic bonding from copper ions upon the reduced graphene oxide based bioinspired nanocomposites, which show the integrated tensile strength, toughness and excellent fatigue-resistant property, as well as high electrical conductivity. These ex- traordinary properties allow this kind of bioinspired nanocomposites to potentially utilize in the fields of aerospace, flexible electronics devices, etc. This study also opens a door for fabricating excellent mechanical performance graphene-based bioin- spired nanocomposites via synergistic interfacial interactions in the future.
基金supported by the National Natural Science Foundation of China(21773128,21534005,and 21421001)。
文摘Nonprecious metal-based oxygen reduction reaction(ORR)electrocatalysts with high efficiency in both alkaline and acidic media are being intensively studied for the purpose of replacing expensive Pt-based catalysts;however,it is still a challenge to achieve superior ORR performances,especially in acidic media.Herein,by pyrolysis of mixed precursors of diammonium phosphate,melamine and hemin,we prepared a nanocomposite catalyst(denoted as FeP@PGL)composed of nitrogen-doped carbon nanosheets with embedded FeP nanoparticles(NPs),which were encapsulated by in-situ formed phosphorus-doped graphene layers.It is found that phosphorous was preferentially doped in the coating layers on FeP NPs,instead of in the carbon nanosheets.The FeP@PGL catalyst exhibited excellent ORR performance,with the onset and half-wave potential up to 1.01 and 0.90 V vs.the reversible hydrogen electrode(RHE)in alkaline media,and0.95 and 0.81 V vs.RHE in acidic media,respectively.By thorough microscopy and spectroscopy characterizations,the interfacial charge transfer between the encapsulated FeP NPs and P-doped graphene layers was identified,and the local work function of the catalyst surface was also reduced by the interfacial interaction.The interfacial synergy between the encapsulated FeP and phosphorus-doped graphene layers was essential to enhance the ORR performance.This study not only demonstrates the promising ORR properties of the encapsulated-FeP-based nanocomposite catalyst,but also provides direct evidence of the interfacial charge transfer effect and its role in ORR process.
基金supported by the National Key R&D Program of China(2020YFB1505802)the Ministry of Science and Technology of China(2017YFA0208200,2016YFA0204100)+4 种基金the National Natural Science Foundation of China(22025108,U21A20327,and22121001)China Postdoctoral Science Foundation(2020M682083)Guangdong Provincial Natural Science Fund for Distinguished Young Scholars(2021B1515020081)Start-up Support from Xiamen University and the Guangzhou Key Laboratory of Low Dimensional Materials and Energy Storage Devices(20195010002)。
文摘Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction(HOR) and hydrogen evolution reaction(HER) due to its similar binding energy towards *H but lower price compared to Pt.Nevertheless, the quest of high-efficiency Ru-based catalysts for HOR and HER is driven by the current disadvantages including low activity and unsatisfactory stability. Herein, we have fabricated and engineered two-dimensional(2D) Ru-based snow-like nanosheets with Ru/Ru O2interface(Ru/Ru O2SNSs)via a post-annealing treatment. Detailed characterizations and theoretical calculations indicate that the interfacial synergy, which is dependent on the temperature for annealing, can alter the hydrogen binding energy(HBE) and hydroxide binding energy(OHBE), as a result of the enhanced HOR and HER performance. Impressively, the optimal Ru/RuO_(2) SNSs display a mass activity of 9.13 A mgRu^(–1) at an overpotential of 50 m V in 0.1 mol L^(–1) KOH for HOR, which is 65, 304, and 21 times higher than those of Ru SNSs(0.14 A mg_(Ru)^(–1)), RuO_(2) SNSs(0.03 A mg_(Ru)^(–1)), and commercial Pt/C(0.43 A mg_(Ru)^(–1)), respectively.Moreover, Ru/RuO_(2) SNSs display improved HER activity with a low overpotential of 20.2 m V for achieving10 m A cm^(-2)in 1 mol L^(–1)KOH. This work not only provides an efficient catalyst for HOR and HER, but also promotes fundamental research on the fabrication and modification of catalysts in heterogeneous catalysis.