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1.
Electrowetting is one approach to reducing the interfacial tension between a solid and a liquid. In this method, an electrical potential is applied across the solid/liquid interface which modifies the wetting properties of the liquid on the solid without changing the composition of the solid and liquid phases. Electrowetting of aligned carbon nanotube (CNT) films is investigated by the sessile drop method by dispensing deionized (DI) water or 0.03 M NaCl droplets (contacted by Au wire) onto aligned CNT films assembled on a copper substrate. The results demonstrate that electrowetting can greatly reduce the hydrophobicity of the aligned CNTs; the contact angle saturation for DI water and 0.03 M NaCl droplets occurs at 98 and 50 degrees , respectively. The combined effects of the geometrical roughness and the electrical potential on the contact angle are briefly discussed and modeled. Such a strategy may be invoked to controllably reduce the interfacial tension between carbon nanotubes (CNTs) and polymer precursors when infiltrating the monomers into the prealigned nanotube films.  相似文献   

2.
Mesoporous multiwalled carbon nanotubes/titanium dioxide (CNTs/TiO(2)) nanocomposites with low loading amounts (0-0.5 wt%) of CNTs embedded inside mesoporous TiO(2) aggregates has been prepared by a simple one-pot hydrothermal method using titanium sulfate as titanium source. The as-prepared CNTs/TiO(2) samples are carefully characterized, analyzed and discussed. In contrast to previous reports with high CNT loading, our results indicate that a low CNT loading slightly influences the textural properties (including crystallite size, degree of crystallinity, specific surface areas, and pore volume etc.) and UV-light absorption of the mesoporous TiO(2) aggregates. The SEM and TEM results demonstrate that the CNTs are mostly embedded in the mesoporous TiO(2) aggregates. Moreover, chemical bonds are formed at the interface between CNTs and TiO(2), which is confirmed by the Raman, IR and XPS analyses. Significantly, we point out that PL analysis in terms of intensity of PL signals seems to not be a reliable way to monitor the recombination rate in the CNTs/TiO(2) composite, due to the quenching effect of CNTs. Instead, the analysis of transient photocurrent responses is introduced, which definitely reflects CNTs as fast electron transfer channels in chemically-bonded CNTs/TiO(2) composites with low CNT loading. Notably, the positive synergy effects of CNTs and TiO(2) depend on both the CNT loading amount and the state of interfacial contacts. In our study, only these chemically bonded CNTs/TiO(2) nanocomposites with appropriate loading amounts (<0.1 wt%) favor the separation of photogenerated electron-hole pairs and decrease their recombination rate and thus display significantly enhanced photocatalytic activity for degrading acetone in air under UV irradiation, as compared with pristine TiO(2) counterparts and commercial P25 photocatalyst. In contrast, a high CNT loading (>0.1 wt%) results in a decrease in photocatalytic activity; a simple mechanical mixing of CNTs and TiO(2) without forming chemical bonds at the interface also results in inferior photocatalytic performance.  相似文献   

3.
Previous investigations have revealed that even long carbon nanotubes (CNTs) retain bond patterns that are characterized by the localization of Clar rings. Even for CNTs with 10 nm length, an alternated, oscillating structure of Clar and Kekulé patterning was also found, indicating that these arrangements may possibly persist for even longer nanotubes, given that they are finite. In the present work, we perform a detailed and comprehensive theoretical study of this phenomenon, in order to find the causes that give rise to these patterns. A complete set of CNTs with different chiralities, diameters (up to 2 nm), lengths (up to 10 nm) and endings (capped, uncapped, and tailored endings) was considered for such purposes. The results indicate that the Clar patterning appears not only on armchair CNTs, but also on those with chiral angle values close to 30°, and this results in a stabilization of the structure, when compared with the uniform, zigzag CNTs. This stabilizing effect points to the causes that underlie the three Nakamura CNT types, resulting as the superposition of structures with a maximal number of Clar rings. Although there is a strict dependence on the border shape, the main cause of the bond patterning in long tubes is to be found in the intrinsic wrapping of each CNT, because the type and number of oscillations present in the longest structures do not depend on the particular length. Nevertheless, the three Nakamura types of armchair tubes appear to subsist beyond the appearance of oscillations, because each of these sets evolves in a different manner, and energy properties that link them together. Apart from the geometry, Clar patterning was investigated through NICS (Nucleus Independent Chemical Shifts) measures, which reveal a connection between the Clar rings and a local concentration of aromaticity.  相似文献   

4.
Electrical resistance (ER) and thermogram measurements were used to evaluate thermal transfer, interfacial and mechanical properties of carbon fiber reinforced thermoplastic polycarbonate composites. Carbon nanotubes (CNTs) were fairly uniformly dispersed in polycarbonates using a solvent dispersion method. The CNTs were then further dispersed with an additional time using a twin screw extruder. The effect of CNT on the mechanical properties of polycarbonate was evaluated using a thin film tensile test. For thermogram to evaluate the transferring temperature the composite was placed on a hotplate and copper wires were inserted in the composite at uniform thickness intervals. Due to the different inherent thermal conductivity of CNT, ER was measured to detect thermal changes in the carbon fiber/CNT-polycarbonate composites. The comparison of interlaminar shear strength (ILSS) was to investigate effects of CNT on mechanical and interfacial properties. The uniform distribution of CNTs affected all of these properties in carbon fiber-reinforced thermoplastic composite. Furthermore, heat transfer and heat release become more rapid with the addition of CNT than the without case.  相似文献   

5.
Poly(L-lactic acid)(PLLA)-based composites exhibit wide applications in many fields.However,most of hydrophilic fillers usually accelerate the hydrolytic degradation of PLLA,which is unfavorable for the prolonging of the service life of the articles.In this work,a small quantity of poly(methyl methacrylate)(PMMA)(2 wt%-10 wt%)was incorporated into the PLLA/carbon nanotubes(CNTs)composites.The effects of PMMA content on the dispersion of CNTs as well as the microstructure and hydrolytic degradation behaviors of the composites were systematically investigated.The results showed that PMMA promoted the dispersion of CNTs in the composites.Amorphous PLLA was obtained in all the composites.Largely enhanced hydrolytic degradation resistance was achieved by incorporating PMMA,especially at relatively high PMMA content.Incorporating 10 wt%PMMA led to a dramatic decrease in the hydrolytic degradation rate from 0.19%/h of the PLLA/CNT composite sample to 0.059%/h of the PLLA/PMMA-10/CNT composite sample.The microstructure evolution of the composites was also detected,and the results showed that no crystallization occurred in the PLLA matrix.Further results based on the interfacial tension calculation showed that the enhanced hydrolytic degradation resistance of the PLLA matrix was mainly attributed to the relatively strong interfacial affinity between PMMA and CNTs,which prevented the occurrence of hydrolytic degradation at the interface between PLLA and CNTs.This work provides an alternative method for tailoring the hydrolytic degradation ability of the PLLA-based composites.  相似文献   

6.
Aligning carbon nanotubes (CNTs) is a key challenge for fabricating CNT‐based electronic devices. Herein, we report a spherical nucleic acid (SNA) mediated approach for the highly precise alignment of CNTs at prescribed sites on DNA origami. We find that the cooperative DNA hybridization occurring at the interface of SNA and DNA‐coated CNTs leads to an approximately five‐fold improvement of the positioning efficiency. By combining this with the intrinsic positioning addressability of DNA origami, CNTs can be aligned in parallel with an extremely small angular variation of within 10°. Moreover, we demonstrate that the parallel alignment of CNTs prevents incorrect logic functionality originating from stray conducting paths formed by misaligned CNTs. This SNA‐mediated method thus holds great potential for fabricating scalable CNT arrays for nanoelectronics.  相似文献   

7.
Multi-walled carbon nanotubes (CNTs) were non-covalently functionalized by surface wrapping of poly(sodium 4-styrenesulfonate) (PSS) with the aid of ultrasound. The functionalized CNTs were incorporated into poly(butylene succinate) (PBS) through solution coagulation to fabricate CNTs filled PBS nanocomposites. The morphologies of the PBS/CNT nanocomposites were studied by scanning electron microscope (SEM) and transmission electron microscope (TEM), and the effect of loading of functionalized CNT on the rheological behavior, electrical conductivity and mechanical properties of the nanocomposites was investigated systemically. SEM observation indicates that functionalized CNTs dispersed in PBS matrix without obvious aggregation and showed good interfacial adhesion with the PBS phase. TEM observation reveals that a CNT network was formed when the loading of CNTs increased from 0.1 to 0.3 wt%. Rheological investigation indicates the formation of a CNT network with a percolation threshold of only 0.3 wt%. Significant improvement in electrical conductivity occurred at CNT loading of 0.3 wt%, with the value of electrical conductivity increasing by six orders of magnitude compared to neat PBS. Differential scanning calorimetry indicates that the melt crystallization temperature of PBS was improved by ∼14 °C with addition of only 0.05 wt% functionalized CNTs. Tensile tests indicate that both the yield strength and Young's modulus of PBS were apparently reinforced by incorporation of functionalized CNTs, while the elongation at break was reduced gradually.  相似文献   

8.
Carbon nanotubes (CNTs) have been widely used in a variety of applications because of their unique structure and excellent mechanical and electrical properties. Additionally, silver (Ag) nanoparticles exhibit broad-spectrum biocidal activity toward many different bacteria, fungi, and viruses. In this study, we prepared Ag-coated CNT hybrid nanoparticles (Ag/CNTs) using aerosol nebulization and thermal evaporation/condensation processes and tested their usefulness for antimicrobial air filtration. Droplets were generated from a CNT suspension using a six-jet collison nebulizer, passed through a diffusion dryer to remove moisture, and entered a thermal tube furnace where silver nanoparticles were generated by thermal evaporation/condensation at ~980 °C in a nitrogen atmosphere. The CNT and Ag nanoparticle aerosols mixed together and attached to each other, forming Ag/CNTs. For physicochemical characterization, the Ag/CNTs were introduced into a scanning mobility particle sizer (SMPS) for size distribution measurements and were sampled by the nanoparticle sampler for morphological and elemental analyses. For antimicrobial air filtration applications, the airborne Ag/CNT particles generated were deposited continuously onto an air filter medium. Physical characteristics (fiber morphology, pressure drop, and filtration efficiency) and biological characteristics (antimicrobial tests against Staphylococcus epidermidis and Escherichia coli bioaerosols) were evaluated. Real-time SMPS and transmission electron microscopy (TEM) data showed that Ag nanoparticles that were <20 nm in diameter were homogeneously dispersed and adhered strongly to the CNT surfaces. Because of the attachment of Ag nanoparticles onto the CNT surfaces, the total particle surface area concentration measured by a nanoparticle surface area monitor (NSAM) was lower than the summation of each Ag nanoparticle and CNT generated. When Ag/CNTs were deposited on the surface of an air filter medium, the antimicrobial activity against test bacterial bioaerosols was enhanced, compared with the deposition of CNTs or Ag nanoparticles alone, whereas the filter pressure drop and bioaerosol filtration efficiency were similar to those of CNT deposition only. At a residence time of 2 h, the relative microbial viabilities of gram-positive S. epidermidis were ~32, 13, 5, and 0.9% on the control, CNT-, Ag nanoparticle-, and Ag/CNT-deposited filters, respectively, and those of gram-negative E. coli were 13, 2.1, 0.4, and 0.1% on the control, CNTs, Ag nanoparticles, and Ag/CNTs, respectively. These Ag/CNT hybrid nanoparticles may be useful for applications in biomedical devices and antibacterial control systems.  相似文献   

9.
Gu  Yaxiong  Chen  Ye  Dong  Yifan  Liu  Junjie  Zhang  Xianhao  Li  Mingzhi  Shao  Yuanhua 《中国科学:化学(英文版)》2020,63(3):411-418
The study of microscopic structure of a liquid/liquid interface is of fundamental importance due to its close relation to the thermodynamics and kinetics of interfacial charge transfer reactions.In this article,the microscopic structure of a non-polarizable water/nitrobenzene(W/NB) interface was evaluated by scanning ion conductance microscope(SICM).Using SICM with a nanometer-sized quartz pipette filled with an electrolyte solution as the probe,the thickness of this type of W/NB interface could be measured at sub-nanometer scale,based on the continuous change of ionic current from one phase to another one.The effects for thicknesses of the non-polarizable W/NB interfaces with different electrolyte concentrations,the Galvani potentials at the interface and the applied potentials on the probe were measured and systematically analyzed.Both experimental setups,that is an organic phase up and an aqueous down,and a reverse version,were employed to acquire the approach curves.These data were compared with those of an ideal polarizable interface under the similar experimental conditions,and several characteristics of non-polarizable interfaces were found.The thickness of a non-polarizable interface increases with the decrease of electrolyte concentration and the increase of applied potential,which is similar to the situation of a polarizable liquid/liquid interface.We also find that the Galvani potential across a non-polarizable interface can also influence the interfacial thickness,this phenomenon is difficult to observe when using polarizable interface.Most importantly,by the comparison of two kinds of liquid/liquid interfaces,we experimentally proved that much more excess ions are gathered in the space charge layer of non-polarizable interfaces than in that of polarizable interfaces.These results are consistent with the predictions of molecular dynamic simulations and X-ray reflectivity measurements.  相似文献   

10.
In order to achieve dramatic improvements in the performance of rubber materials, the development of carbon nanotube (CNT)‐reinforced rubber composites was attempted. The CNT/natural rubber (NR) nanocomposite was prepared through solvent mixing on the basis of pretreatment of CNTs. Thermal properties, vulcanization characteristics, and physical and mechanical properties of the CNT/NR nanocomposites were characterized in contrast to the carbon black (CB)/NR composite. Through the addition of the CNTs treated using acid bath followed by ball milling with HRH (hydrated silica, resorcinol, and hexamethylene tetramine) bonding systems, the crystallization melting peak in differential scanning calorimetry (DSC) curves of NR weakened and the curing rate of NR slightly decreased. Meanwhile, the over‐curing reversion of CNT/NR nanocomposites was alleviated. The dispersion of the treated CNTs in the rubber matrix and interfacial bonding between them were rather good. The mechanical properties of the CNT‐reinforced NR showed a considerable increase compared to the neat NR and traditional CB/NR composite. At the same time, the CNT/NR nanocomposites exhibited better rebound resilience and dynamic compression properties. The storage modulus of the CNT/NR nanocomposites greatly exceeds that of neat NR and CB/NR composites under all temperature regions. The thermal stability of NR was also obviously improved with the addition of the treated CNTs. Copyright © 2008 John Wiley & Sons, Ltd.  相似文献   

11.
Electron field-emission measurements on individual carbon nanotubes (CNTs) were performed inside the transmission electron microscope (TEM). The field-emission characteristics of CNTs with different tip structures were compared, and their field conversion factor and emission area were studied systematically. It was found that the field-emission characteristics of a CNT depend sensitively on its tip structure, and in particular an opened CNT was shown to be superior to a capped CNT. High-resolution TEM observations revealed that the tip of an opened CNT may, in general, be regarded as being composed of irregular shaped graphitic sheets, and these graphitic sheets have been found to improve dramatically the field-emission characteristics, but the sharp edge may result in larger error in the calculated emission area. The influence of uncertainty in the work function of the CNTs on the field conversion factor and emission area calculation was also investigated.  相似文献   

12.
Aligning carbon nanotubes (CNTs) is a key challenge for fabricating CNT-based electronic devices. Herein, we report a spherical nucleic acid (SNA) mediated approach for the highly precise alignment of CNTs at prescribed sites on DNA origami. We find that the cooperative DNA hybridization occurring at the interface of SNA and DNA-coated CNTs leads to an approximately five-fold improvement of the positioning efficiency. By combining this with the intrinsic positioning addressability of DNA origami, CNTs can be aligned in parallel with an extremely small angular variation of within 10°. Moreover, we demonstrate that the parallel alignment of CNTs prevents incorrect logic functionality originating from stray conducting paths formed by misaligned CNTs. This SNA-mediated method thus holds great potential for fabricating scalable CNT arrays for nanoelectronics.  相似文献   

13.
The recently reported photoswitching of diarylethene derivative molecules bridging carbon nanotube (CNT) contacts is theoretically analyzed. The short lifetime of the lowest unoccupied molecular orbital (LUMO) indicates that neither the open nor closed form of the molecule can be photoexcited into a charge-neutral excited state for any appreciable length of time preventing photochromic ring opening. Analysis of the highest occupied molecular orbital (HOMO) and LUMO lifetimes also suggests that photoexcitation results in oxidation of the molecules. This either reduces the quantum yield of photochromic ring closing, or it gives rise to the possibility of oxidative ring closing. Analysis of the resistance values and energy levels indicates that the HOMO energy levels of the closed isomers relevant for transport must lie within a few k(B)T of the CNT Fermi level. For armchair contacts, the change in resistance with isomer or substituent group is the result of shifts in the energy level of the molecular HOMO. The coupling of the molecular HOMO to the CNT contacts is insensitive to the isomer type or substituent group. For zigzag CNTs, the conductance is dominated by surface states at the Fermi level on the cut ends of the CNTs so that the conductance is relatively insensitive to the isomer type, and the conductance switching ratio is low. Multiple bridging molecules can interact coherently, resulting in energy splitting, shifting, and interference that cause a nonlinear change in conductance with increasing numbers of molecules. Instead of a factor of 3 increase in conductance expected for three independent channels, a factor of 10(3) increase in conductance is obtained for three bridging molecules.  相似文献   

14.
PBEPBE‐D3 calculations were performed to investigate how platinum (Pt) interacts with the internal and external surfaces of single‐walled pristine, Si‐, Ge‐, and Sn‐doped (6,6) carbon nanotubes (CNTs). Our calculations showed that atomic Pt demonstrates stronger binding strength on the external surfaces than the internal surface adsorption for the same type of nanotube. In cases of external surface adsorptions, Si‐, Ge‐, and Sn‐doped CNTs show comparable binding energies for Pt, at least 1.40 eV larger than pristine CNT. This enhancement can be rationalized by the strong covalent interactions between Pt and X? C (X = Si, Ge, and Sn) pairs based on structural and projected density of states analysis. In terms of internal surface adsorptions, Ge and Sn doping could significantly enhance the binding of Pt. Pt atom shows much more delocalized and bonding states inside Ge‐ and Sn‐doped CNTs, indicating multiple‐site interaction pattern when atomic Pt is confined inside the nanotubes. However, the internal surface of Si‐doped CNT presents limited enhancement in Pt adsorption with respect to that of pristine CNT because of their similar binding geometries. © 2016 Wiley Periodicals, Inc.  相似文献   

15.
We present a systematic study of atmospheric chemical vapor deposition growth of carbon nanotubes (CNTs) on patterned, transition metal/GaAs samples employing methane as the carbon feedstock. Controlled CNT growth was found to occur from the exposed metal‐semiconductor interface, rather than from the metal or semiconductor surfaces themselves. A fast sample loading system allowed for a minimization of the exposure to high temperatures, thereby preventing excessive sample damage. The optimum growth temperature for CrNi/GaAs interfaces is 700 °C (at a methane flow rate of 700 sccm). Possible growth scenarios involving the Ni–As–Ga system and its interaction with C is discussed. Raman spectroscopy of the CNTs revealed the presence of pentagon–heptagon defects. Closer analysis of the spectra points towards a mixture of so‐called Haeckelite CNTs. Copyright © 2011 John Wiley & Sons, Ltd.  相似文献   

16.
The adhesion of copper films to adjacent device layers including TiN, Ta, and TaN diffusion barriers is a crucial reliability issue for integrated circuits. We report that ultrathin layers of poly(acrylic acid) (PAA) prepared on barrier surfaces or on the native oxide of Si wafers dramatically increase the interfacial adhesion of Cu films deposited by the H2 assisted reduction of bis(2,2,7-trimethyloctane-3,5-dionato)copper in supercritical carbon dioxide. Similar improvements were achieved on Si wafers using a simple vapor phase exposure of the substrate to acrylic acid prior to metallization. The deposited films and the substrate/Cu interfaces were analyzed by X-ray photoelectron spectroscopy (XPS), electron microscopy, atomic force microscopy, and variable-angle spectroscopic ellipsometry. No trace of the adhesion layer was detected at the interface, indicating it was sacrificial at the deposition conditions used. Moreover, the presence and subsequent decomposition of the PAA layer during deposition substantially reduced or eliminated metal oxides at the substrate interface. For depositions on PAA-treated Si wafers, copper was present primarily as Cu0 at the interface and Si was present only as Si0. On PAA-treated Ta substrates, XPS analysis indicated Ta was present primarily as Ta0 at the metallized interface whereas Ta2O5 dominated the interface of samples prepared without the adhesion layers. The technique can be extended to patterned substrates using adsorption of acrylic acid or thermal/UV polymerization of acrylic acid.  相似文献   

17.
The rheological behavior of beta-casein adsorption layers formed at the air-water and tetradecane-water interfaces is studied in detail by means of pendant drop tensiometry. First, its adsorption behavior is briefly summarized at both interfaces, experimentally and also theoretically. Subsequently, the experimental dilatational results obtained for a wide range of frequencies are presented for both interfaces. An interesting dependence with the oscillation frequency is observed via the comparative analysis of the interfacial elasticity (storage part) and the interfacial viscosity (loss part) for the two interfaces. The analysis of the interfacial elasticities provides information on the conformational transitions undergone by the protein upon adsorption at both interfaces. The air-water interface shows a complex behavior in which two maxima merge into one as the frequency increases, whereas only a single maximum is found at the tetradecane interface within the range of frequencies studied. This is interpreted in terms of a decisive interaction between the oil and the protein molecules. Furthermore, the analysis of the interfacial viscosities provides information on the relaxation processes occurring at both interfaces. Similarly, substantial differences arise between the gaseous and liquid interfaces and various possible relaxation mechanisms are discussed. Finally, the experimental elasticities obtained for frequencies higher than 0.1 Hz are further analyzed on the basis of a thermodynamic model. Accordingly, the nature of the conformational transition given by the maximum at these frequencies is discussed in terms of different theoretical considerations. The formation of a protein bilayer at the interface or the limited compressibility of the protein in the adsorbed state are regarded as possible explanations of the maximum.  相似文献   

18.
We present a neutron reflectivity study on interfaces in contact with flowing hexadecane, which is known to exhibit surface slip on functionalized solid surfaces. The single crystalline silicon substrates were either chemically cleaned Si(100) or Si(100) coated by octadecyl-trichlorosilane (OTS), which resulted in different interfacial energies. The liquid was sheared in situ and changes in reflectivity profiles were compared to the static case. For the OTS surface, the temperature dependence was also recorded. For both types of interfaces, density depletion of the liquid at the interface was observed. In the case of the bare Si substrate, shear load altered the structure of the depletion layer, whereas for the OTS covered surface no effect of shear was observed. Possible links between the depletion layer and surface slip are discussed. The results show that, in contrast to water, for hexadecane the enhancement of the depletion layer with temperature and interfacial energy reduces the amount of slip. Thus a density depletion cannot be the origin of surface slip in this system.  相似文献   

19.
Carbon nanotubes (CNTs) were grown directly on the surface of carbon fibres, using the catalytic chemical vapour deposition. FeCo bimetallic catalysts were deposited on carbon fibres using a simple wet impregnation method. CNTs were synthesized over the prepared catalysts by the catalytic decomposition of acetylene at 750oC. The uniform CNT formation on the fibre surface was verified using scanning electron microscopy. Raman spectroscopy was employed to evaluate non‐destructively the CNT growth and the CNT quality. Thermo gravimetric analysis and differential thermal analysis were employed as destructive methods to confirm the spectroscopic data. Single CNT‐coated fibre fragmentation tests were performed to examine the interfacial shear strength (ISS) of the modified fibres. Acoustic emission was employed to monitor the fragmentation process in real time. Thus, the coated fibre structural integrity was assessed together with its stress transfer properties. Polarized optical microscopy was employed to cross validate the acoustic emission data. It was found that the ISS of the nanotube‐reinforced interphase was improved without affecting the fibre mechanical properties. Copyright © 2013 John Wiley & Sons, Ltd.  相似文献   

20.
The adsorption behavior of dioctyldimethylammonium chloride at water/ hexane interface has been studied by measuring the interfacial tension as a function of temperature and pressure at various bulk concentrations. By applying the thermodynamics of adsorption at interfaces to the experimental results, the thermodynamic quantity changes associated with adsorption and the interfacial density of dioctyldimethylammonium chloride have been evaluated.The interfacial tension vs temperature and concentration curves have shown the breaks and it has been concluded that the first order phase transition takes place between a gaseous and an expanded state. The entropy and volume changes associated with adsorption have shown the remarkable dependence on temperature and pressure and have been found to decrease with increasing the molality. Also the energy change associated with adsorption has been evaluated and it has been concluded that the adsorption of dioctyldimethylammonium chloride at water/hexane interface is enhanced by negative values of the partial molar energy change. Further, all the thermodynamic quantities have been characterized by the discontinuous change attributable to the phase transition.  相似文献   

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