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1.
Conducting polypyrrole (PPy) and poly(pyrrole-2,6-dimethyl-β-cyclodextrin) [poly(Py-β-DMCD)] films were prepared by electrode
potential cycling on a gold electrode in aqueous and nonaqueous (acetonitrile) electrolyte solutions containing lithium perchlorate.
The resulting products were characterized with cyclic voltammetry, in situ UV–Vis spectroscopy, and in situ conductivity measurements.
For the electrosynthesis of poly(Py-β-DMCD), a (1:1) (mole–mole) (Py-β-DMCD) supramolecular cyclodextrin complex of pyrrole
previously characterized with proton NMR spectroscopy was used as starting material. A different cyclic voltammetric behavior
was observed for pyrrole and the poly(Py-β-DMCD) complex in aqueous and nonaqueous solutions during electrosynthesis. The
results show that in both solutions in the presence of cyclodextrin, the oxidation potential of pyrrole monomers increases.
However, the difference of oxidation potentials for films prepared in aqueous solution is larger than for the films prepared
in nonaqueous solution. In situ conductivity measurements of the films show that films prepared in acetonitrile solution are
more conductive than those synthesized in aqueous solutions. Maximum conductivity can be observed for PPy and poly(Py-β-DMCD)
films prepared in nonaqueous solution in the range of 0.10 < E
Ag/AgCl < 0.90 V and 0.30 < E
Ag/AgCl < 0.90 V, respectively. In situ UV–Vis spectroelectrochemical data for both films prepared potentiodynamically by cycling
the potentials from −0.40 < E
Ag/AgCl < 0.90 V in nonaqueous solutions are reported.
This paper is dedicated to Prof. Alan Bond on the occasion of his 65th birthday in recognition of his numerous contributions
toward electrochemistry. 相似文献
2.
In this work, polypyrrole films with ferrocenecarboxylic acid incorporated (PPy/FCA) were prepared on a glassy carbon (GC)
electrode in chloroform as an aprotic solvent with low dielectric constant, convenient for the preparation of the films by
a precipitation mechanism. The electrochemical behaviour of the PPy/FCA-coated GC electrode was studied by cyclic voltammetry
in aqueous solution with low pH. The results obtained show that the electrochemical response of FCA incorporated in polypyrrole
is consistent with a reversible surface oxidation. An obvious electrocatalytic effect of PPy/FCA on the oxidation of ascorbic
acid is observed in aqueous solution.
Received: 30 July 1998 / Accepted: 3 March 1999 相似文献
3.
C. Perruchot M. M. Chehimi M. Delamar E. Cabet-Deliry B. Miksa S. Slomkowski M. A. Khan S. P. Armes 《Colloid and polymer science》2000,278(12):1139-1154
Thin chloride-doped polypyrrole films (PPyCl) were deposited chemically onto untreated and silane-treated planar glass plates
from aqueous solutions. The organosilanes used to treat the glass substrates were methyltriethoxysilane (Cl), propyltrimethoxysilane
(C3), octyltrimethoxysilane (C8) and aminopropyltriethoxysilane (APS). The decreasing order of hydrophobic character of silane-treated
glass slides, as measured by water contact angle measurements, was glass–APS ≅ glass–C8 > glass–C3 > glass–C1 > glass. X-ray
photoelectron spectroscopy was used to determine the surface chemical composition of the glass plates before and following
coating with the silane coupling agents and/or the PPy thin layer, respectively. The attenuation in intensity of the glass
Na1
s
peak enabled the average thickness of the various organosilane overlayers to be estimated. Atomic force microscopy showed
that the morphology of the organosilane overlayers was islandlike. The domains have a structure which depends upon the nature
of the organosilane in question. Scanning electron microscope images showed that the morphology of the PPyCl thin films was
homogeneous when coated onto glass–APS and glass–C8, but wrinkled at the surface of glass, glass–C1 and glass–C3 plates. Qualitative
peel tests using 3M adhesive tape showed very good adhesion of PPyCl to the glass–APS substrate, whereas adhesion was fairly
poor in the case of glass–PPy and PPy–alkylsilane–glass interfaces. The results of this multitechnique study suggest that
hydrophobic interactions are important to obtain homogeneous and continuous thin PPy films, but Lewis acid–base interactions
are the driving forces for strong and durable PPy–glass adhesion.
Received: 3 January 2000/Accepted: 19 May 2000 相似文献
4.
Polypyrrole (PPy)-coated poly(vinyl chloride) (PVC) powder particles were prepared by the in situ chemical polymerisation of pyrrole in aqueous solutions in the presence of PVC powder particles. The PVC particles in suspension served as a hydrophobic substrate for the in situ polymerisation of pyrrole using iron chloride as the oxidising agent and sodium p-toluene sulfonate. In these conditions, tosylate-doped PPy (PPyTS) was obtained and chlorides were inserted as minor codoping species. In some cases, the pyrrole was polymerised after incubating the PVC particles with poly(N-vinyl pyrrolidone). Scanning electron microscope (SEM) micrographs showed that the PVC particles retained their initial, quasispherical shape after coating by PPy. At low magnification, the coated PVC particles appeared smooth, but at high magnification, they exhibited a decoration by elementary nanoparticles of about 200-nm size due to PPy bulk powder grains. Elemental analysis indicated a mass loading of PPy in the range 1–58% w/w. Specific surface analysis by X-ray photoelectron spectroscopy (XPS) resulted in the spectra of the PPy-coated PVC particles resembling those of bulk powder PPyTS even for low PPy mass loading. The surface fraction of PPy repeat units was found to vary in the 55–91% range. This result is consistent with the SEM observation of the PPy nanoparticles at the surface of PVC powder grains. However, despite the important loading of PPy, the XPS estimation of the overlayer thickness is in favour of a patchy coating rather than continuous coatings of PPy. 相似文献
5.
The effect of chloride concentration and pH on pitting corrosion of AA7075 aluminum alloy coated with phenyltrimethoxysilane 总被引:1,自引:0,他引:1
A. A. Younis M. M. B. El-Sabbah Rudolf Holze 《Journal of Solid State Electrochemistry》2012,16(3):1033-1040
The effect of chloride ion concentration and pH of solution on the corrosion behavior of aluminum alloy AA7075 coated with
phenyltrimethoxysilane (PTMS) immersed in aqueous solutions of NaCl is reported. Potentiodynamic polarization, linear polarization,
open circuit potential, and weight loss measurements were performed. The surface of samples was examined using SEM and optical
microscopy. Elemental characterization of the coating by secondary ion mass spectrometry indicates an intermediate layer between
coating and aluminum alloy surface. The corrosion behavior of the aluminum alloy AA7075 depends on chloride concentration
and pH of solution. In acidic or neutral solutions, general and pitting corrosion occur simultaneously. On the contrary, exposure
to alkaline solutions results in general corrosion only. Results further reveal that aluminum alloy AA7075 is susceptible
to pitting corrosion in all chloride solutions with concentrations between 0.05 M and 2 M NaCl; an increase in the chloride
concentration slightly shifted both the pitting and corrosion potentials to more active values. Linear polarization resistance
measurements show a substantially improved corrosion resistance value in case of samples coated with PTMS as compared to uncoated
samples in both neutral (pH = 7), acidic (pH = 0.85 and 3), and alkaline chloride solutions (pH = 10 and 12.85). The higher
corrosion resistance of the aluminum alloy coated with PTMS can be attributed to the hydrophobic coating which acts as a barrier
and prevents chloride ion penetration and subsequent reaction with the aluminum alloy. 相似文献
6.
A highly sensitive hydroxylamine (HA) electrochemical sensor is developed based on electrodeposition of gold nanoparticles
with diameter of 8 nm on the pre-synthesized polypyrrole matrix and formed gold nanoparticles/polypyrrole (GNPs/PPy) composite
on glassy carbon electrode. The electrochemical behavior and electrocatalytic activity of the composite-modified electrode
are investigated. The GNPs/PPy composite exhibits a distinctly higher electrocatalytic activity for the oxidation of HA than
GNPs with twofold enhancement of peak current. The enhanced electrocatalytic activity is attributed to the synergic effect
of the highly dispersed gold metal particles and PPy matrix. The overall numbers of electrons involved in HA oxidation, the
electron transfer coefficient, catalytic rate constant, and diffusion coefficient are investigated by chronoamperometry. The
sensor presents two wide linear ranges of 4.5 × 10−7–1.2 × 10−3 M and 1.2 × 10−3–19 × 10−3 M with the detection limit of 4.5 × 10−8 M (s/n = 3). In addition, the proposed electrode shows excellent sensitivity, selectivity, reproducibility, and stability properties. 相似文献
7.
Pure metallic Cu nanoparticles at a high concentration (up to 0.2 M) have been synthesized by the reduction of cupric chloride with hydrazine in the aqueous CTAB solution. The input of extra inert gases was not necessary. The use of ammonia solution for the adjustment of solution pH up to 10 and the use of hydrazine as a reducing agent in a capped reaction bottle are crucial for the synthesis of pure Cu nanoparticles. The reaction solution finally became wine-reddish and its UV/vis absorption spectrum exhibited an absorption band at 574 nm, revealing the formation of metallic Cu nanoparticles. By the analysis of electron diffraction pattern, EDS, XRD, and XPS, the resultant particles were confirmed to be pure Cu with a face-centered cubic (fcc) structure. From the TEM analysis, it was found that the mean diameter of Cu nanoparticles first decreased and then approached a constant with the increase of hydrazine concentration. In addition, the CTAB concentration had not significant influence on the size of Cu nanoparticles. Also, TG analysis indicated that there were two weight-loss steps for the CTAB-capped Cu nanoparticles. It was suggested that a bilayer structure of CTAB was formed on the surface of Cu nanoparticles to prevent from the particle agglomeration. The synthesis method reported in this work might be helpful for the large-scale production of Cu nanoparticles. 相似文献
8.
Core–shell latex particles made of a poly(butyl methacrylate) (PBMA) core and a thin polypyrrole (PPy) shell were synthesized
by two-stage polymerization. In the first stage, PBMA latex particles were synthesized in a semicontinuous process by free-radical
polymerization. PBMA latex particles were labeled either with an energy donor or with an energy acceptor, in two different
syntheses. These particles were used in a second stage as seeds for the synthesis of the core–shell particles. The PPy shell
was polymerized around the PBMA core latex in an oxidative chemical in situ polymerization. Proofs for the success of the
core–shell synthesis were obtained using nonradiative energy transfer (NRET) and atomic force microscopy (AFM). NRET gives
access to the rate of polymer chain migration between adjacent particles in a film annealed at a temperature above the glass-transition
temperature T
g of the particles. Slower chain migration of the PBMA polymer chains was obtained with the PBMA–PPy core–shell particles compared
to rate of the PBMA polymer chain migration found with the pure, uncoated PBMA particles. This result is due to the coating
of PBMA by PPy, which hinders the migration of the PBMA polymer chains between adjacent particles in the film. This observation
has been confirmed by AFM measurements showing that the flattening of the latex film surface is much slower for the core–shell
particles than for the pure PBMA particles. This result can again be explained by the presence of a rigid PPy shell around
the PBMA core. Thus, these two complementary methods have given evidence that real core–shell particles were synthesized and
that the shell seriously hinders film formation of the particles in spite of the fact that it is very thin (thickness close
to 1 nm) compared to the size (750 and 780 nm in diameter) of the PBMA core. Transparency measurements confirm the results
obtained by NRET and AFM. When the films are placed at a temperature higher than the T
g of PBMA, the increase in transparency is faster for films made with the uncoated PBMA particles than for films made with
the coated PBMA particles. This result indicates again that the presence of the rigid PPy layer around the PBMA core reduces
considerably the speed at which the structure of the film is modified when heated above the T
g of PBMA.
Received: 02 September 1999 Accepted: 21 December 1999 相似文献
9.
Edit Pál Robert Kun Christina Schulze Volker Z?llmer Dirk Lehmhus Marcus B?umer Matthias Busse 《Colloid and polymer science》2012,290(10):941-952
Copper, nickel and copper–nickel nanoparticles were prepared by solution combustion method for use in direct write printing. Structural (X-ray diffraction) and morphological (transmission electron microscope) investigations showed that pure metal (Cu and Ni) and CuNi alloy particles with face-centred cubic crystal structure were formed. Atomic absorption spectrometer studies confirmed that the nanoparticle compositions corresponded to the initial Cu/Ni molar ratios selected for synthesis. Particle size and morphology were significantly influenced by composition, with high Cu content coinciding with small, spherical particles as opposed to larger, irregular shapes observed at high Ni concentrations. X-ray photoelectron spectroscopy measurements revealed that after the reduction process the surface of the alloy nanoparticles was partially oxidised in air and the amount of metallic surface species decreased, while the concentration of oxidic surface species and hydroxides increased with increasing Cu concentration (i.e. decreasing particle size). Dispersions of CuNi nanoparticles have been deposited by use of AerosolJet? and sintered under reducing atmosphere at 300–800?°C in order to prepare conductive structures. Resistivity measurements and microscopical studies (SEM-FIB) of printed and sintered CuNi structures showed that the sintering properties of nanoparticles were dependent on their chemical composition. 相似文献
10.
Azizollah Nezhadali 《Journal of inclusion phenomena and macrocyclic chemistry》2006,54(3-4):307-308
The selective polymer membrane transport of Cu(II) from an aqueous solution containing seven metal cations, Co(II), Ni(II), Cu(II), Zn(II), Ag(II), Cd(II) and Pb(II), was studied .The source phase contained equimolar concentrations of the above-mentioned cations, with the source and receiving phases being buffered at pH 4.9 and 3.0, respectively. Cu(II) ion transport occurred (J=2.82 × 10−7 mol/h at 25 °C) from the aqueous source phase across the polymer membrane (derived from cellulose triacetate) containing ligand (I) as the ionophore, into the aqueous receiving phase. Clear transport selectivity for Cu(II) was observed. 相似文献
11.
A fiber-packed needle was developed as a novel extraction device for gas-chromatographic analysis of trace organic compounds
in aqueous samples. In the extraction device, a bundle of the polymer-coated filaments as the sorbent material was longitudinally
packed into a specially designed needle. The extraction was made by pumping the aqueous sample solution into the needle extraction
device, and the subsequent desorption process was carried out with a flow of desorption solvent through the needle in a heated
gas chromatograph injector. The needle device showed an excellent thermal stability for repeated use without any deterioration
of extraction performance, and no carryover effect was observed after the optimization of the desorption conditions. Additionally,
the extraction efficiency of the fiber-packed needle could be enhanced by optimizing the number of packed filaments. The selectivity
for various compounds could be also tuned using an appropriate combination of the fibrous medium and the coating polymer.
The relative standard deviation for run to run was from 3.88 to 4.55% (n = 5), and that for needle to needle was 7.21% (n = 3), clearly suggesting a good repeatability of the needle extraction technique developed. Upon successful optimization
of the extraction conditions, a rapid extraction of trace organic compounds from an aqueous sample matrix was successfully
demonstrated, where each extraction process was completed within 10 min. 相似文献
12.
Jakub Čížek Ivan Procházka Radomír Kužel Rinat K. Islamgaliev 《Monatshefte für Chemie / Chemical Monthly》2002,133(6):873-887
Summary. Ultra-fine grained (UFG) Cu (grain size 80 nm) containing 0.5 wt.% Al2O3 nanoparticles (size 20 nm) was prepared by high pressure torsion (HPT). Positron lifetime spectroscopy was employed to characterize
the microstructure of this material, especially with respect to types and concentration of lattice defects. The evolution
of microstructure with increasing temperature was studied by positron lifetime spectroscopy and X-ray diffraction measurements.
The thermal stability of the Cu + 0.5 wt.% Al2O3 nanocomposite was compared with that of pure UFG Cu prepared by the same technique. The processes taking place during thermal
recovery of the initial nanoscale structure in both studied materials are described.
Received October 5, 2001. Accepted (revised) December 20, 2001 相似文献
13.
Polychloromethylstyrene nanoparticles of sizes from 12.0 ± 2.3 to 229.6 ± 65 nm were prepared by the emulsion and miniemulsion
polymerization of chloromethylstyrene in an aqueous continuous phase in the presence of potassium persulfate as initiator,
sodium octylbenzenesulfonate as surfactant, and hexadecane as costabilizer for the miniemulsion polymerization process only.
The influence of various polymerization parameters (e.g., concentration of the monomer, initiator, the crosslinker monomer,
and the surfactant) on the properties of the particles (e.g., size, size distribution, and yield) has been elucidated. The
polychloromethylstyrene nanoparticles formed via the emulsion polymerization mechanism possess smaller diameter and size distribution
than those formed under similar conditions via the miniemulsion polymerization mechanism. Other differences between these
two polymerization mechanisms have also been elucidated. For future study, we wish to use these nanoparticles for the covalent
immobilization of bioactive reagents such as proteins to the surface of these nanoparticles for various biomedical applications. 相似文献
14.
Donald A. Palmer 《Journal of solution chemistry》2011,40(6):1067-1093
The equilibrium solubility of crystalline cuprous oxide, cuprite, was measured in liquid water and steam using two flow-through
reactors and a conventional batch autoclave. These measurements were carried out from 20 to 400 °C. Different batches of pretreated
cuprite were thoroughly characterized prior to and following each set of experiments. Metallic copper beads were added to
the inlet end of the reactors and to the solid charge in the autoclave to preserve the Cu(I) oxidation state, although one
series of experiments produced some results which were only compatible with CuO(cr) as the solubility limiting phase. Comparison
of the solubility data for Cu2O(cr) in aqueous solution with those from the only available high-temperature dataset (Var’yash, Geochem. Int. 26:80–90, 1989) showed that in near-neutral solutions the new data are lower by about four orders of magnitude at 350 °C. Moreover, the
dominant species in solution at temperatures ≥100 °C were found to be only Cu+ and Cu(OH)2-\mathrm{Cu(OH)}_{2}^{-} with Cu(OH)0 occurring over a narrow pH range at ≤75 °C rather than the reverse trend reported previously. Solubility equations were developed
as a function of temperature and pH, based on these new results, which showed increased solubility with temperature in acidic
and basic solutions. The solubility of Cu2O(cr) in steam decreased slightly with temperature and as expected increased with increasing pressure to supercritical conditions
where limited, compatible data were available in the literature. The solubility at subcritical conditions was on the order
of one to several parts per billion, ppb. A simple empirical fit was derived for the solubility in steam as a function of
temperature and pressure. 相似文献
15.
Urška L. Štangar Urh Černigoj Polonca Trebše Ksenija Maver Silvia Gross 《Monatshefte für Chemie / Chemical Monthly》2006,137(5):647-655
Summary. Transparent TiO2 films with a high photodegradation activity towards an azo dye in aqueous solution were prepared by sol–gel processing. Films
on soda–lime glass supports protected with a thin silica barrier layer exhibited better crystallization and monodisperse nanoparticles,
higher absorption of light below 370 nm, and higher photocatalytic activity than those films deposited on bare glass supports
proving the detrimental effect of interdiffused sodium ions on the development of the anatase nanostructure. The effect of
substrate was more pronounced in thinner films (300 nm) than in thicker ones (1200 nm), which were achieved by adding a template
(i.e. Pluronic F127) to the sol. 相似文献
16.
Ur?ka L. ?tangar Urh ?ernigoj Polonca Treb?e Ksenija Maver Silvia Gross 《Monatshefte für Chemie / Chemical Monthly》2006,1(6):647-655
Transparent TiO2 films with a high photodegradation activity towards an azo dye in aqueous solution were prepared by sol–gel processing. Films
on soda–lime glass supports protected with a thin silica barrier layer exhibited better crystallization and monodisperse nanoparticles,
higher absorption of light below 370 nm, and higher photocatalytic activity than those films deposited on bare glass supports
proving the detrimental effect of interdiffused sodium ions on the development of the anatase nanostructure. The effect of
substrate was more pronounced in thinner films (300 nm) than in thicker ones (1200 nm), which were achieved by adding a template
(i.e. Pluronic F127) to the sol. 相似文献
17.
Héctor Rosas Leidy Erika Sarmiento Vito Lubes María Goncalves Mary Lorena Araujo Felipe Brito 《Journal of solution chemistry》2008,37(5):701-711
The complex species formed between vanadium(III) cysteine and small blood serum bioligands: lactic, oxalic, citric and phosphoric
acids were studied in aqueous solution by means of electromotive force measurements, Emf(H), at 25 °C and 3.0 mol⋅dm−3 KCl as the ionic medium. The ternary complexes were studied by potentiometric measurements and the data analyzed using the
least-squares computational program LETAGROP to obtain the respective stability constants and stoichiometric coefficients.
The UV-Vis spectrophotometric measurements were done in order to make a qualitative characterization of the complexes formed
in aqueous solution. 相似文献
18.
Conducting polymer poly(pyrrole) (PPy) doped with Nafion was successfully used as ion-to-electron transducer in the construction
of a solid-contact Pb2+-selective polymeric membrane electrode. The Nafion dopant can effectively increase the capacitance of the conducting polymer
and improve the mechanical robustness of the coating. The transducer layer, PPy-Nafion, characterized by cyclic voltammetry
and electrochemical impedance spectroscopy, exhibits a sufficiently high bulk (redox) capacitance and fast ion and electron
transport process. The new Pb2+-selective polymeric membrane electrode, based on PPy-Nafion film as solid contact, shows stable Nernstian characteristics
in Pb(NO3)2 solution within the concentration range of 1.0 × 10−7–1.0 × 10−3 M, and the detection limit is 4.3 × 10−8 M. The potential stability of the electrode and the influence of the interfacial water layer were also evaluated by chronopotentiometry
and potentiometric water layer test, respectively. The results show that the solid-contact Pb2+-selective electrode, based on PPy-Nafion film as ion-to-electron transducer, can effectively overcome the potential drift
and reduce the water layer between the PPy-Nafion transducer layer and the ion-selective membrane. 相似文献
19.
Pinheiro SC Descalzo AB Raimundo IM Orellana G Moreno-Bondi MC 《Analytical and bioanalytical chemistry》2012,402(10):3253-3260
This paper describes the synthesis and characterization of a fluorescent ion-imprinted polymer (IIP) for selective determination
of copper ions in aqueous samples. The IIP has been prepared using a novel functional monomer, 4-[(E)-2-(4′-methyl-2,2′-bipyridin-4-yl)vinyl]phenyl methacrylate (abbreviated as BSOMe) that has been spectroscopically characterized
in methanolic solution, in the absence and in the presence of several metal ions, including Cd(II), Cu(II), Hg(II), Ni(II),
Pb(II), and Zn(II). The stability constant (2.04 × 108 mol−2 l2) and stoichiometry (L2M) of the BSOMe complex with Cu(II) were extracted thereof. Cu(II)-IIPs were prepared by radical polymerization using stoichiometric
amounts of the fluorescent monomer and the template metal ion. The resulting cross-linked network did not show any leaching
of the immobilized ligand allowing determination of Cu(II) in aqueous samples by fluorescence quenching measurements. Several
parameters affecting optosensor performance have been optimized, including sample pH, ionic strength, or polymer regeneration
for online analysis of water samples. The synthesized Cu(II)-IIP exhibits a detection limit of 0.04 μmol l−1 for the determination of Cu(II) in water samples with a reproducibility of 3%, exhibiting an excellent selectivity towards
the template ion over other metal ions with the same charge and close ionic radius. The IIP-based optosensor has been repeatedly
used and regenerated for more than 50 cycles without a significant decrease in the luminescent properties and binding affinity
of the sensing phase. 相似文献
20.
Giorgio Papeschi Stefano Mancuso Anna Maria Marras 《Journal of Solid State Electrochemistry》2000,4(6):325-329
The electrochemical behaviour of a Cu/CuSe electrode was studied in order to define its selectivity towards cupric ions,
Nerstian response, limit of detection and response time. The chalcogenide electrode was prepared by cathodic deposition of
Se and subsequent formation of a thin layer of CuSe on a copper substrate. A Cu/CuSe microelectrode was prepared using copper
wire 75 μm in diameter. The dimensions and response time (<0.5 s) allowed use of this electrode in the “vibrating probe method”
with the aim of measuring net influxes as well as effluxes of copper(II) ions in Olea europaea roots. The electrode potential was measured along the root at a distance of 5 μm from the surface for 5 s, and then again
for 5 s at a distance of 55 μm, moving the microelectrode with respect to the root surface by steps with a frequency of 0.1 Hz.
The potentials measured at the two extremes of vibration were then converted to copper(II) concentrations. Substitution of
these values in Fick's law yields the flux, assuming the diffusion constant D for copper ions in aqueous solutions. The results enabled us to detect copper(II) fluxes as small as 0.05 pmol cm−2 s−1. Copper(II) influx showed marked spatial and temporal features: it was highest at about 1.5 mm from the root apex and exhibited
an oscillatory pattern in time.
Received: 29 September 1999 / Accepted: 11 January 2000 相似文献