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F Ariese

Publications and source records attributed to F Ariese.

At least 19 recordsLinked to original sources

Cavity ring-down spectroscopy for detection in liquid chromatography: extension to tunable sources and ultraviolet wavelengths.

In earlier studies, it was demonstrated that the sensitivity of absorbance detection in liquid chromatography (LC) can be improved significantly by using cavity ring-down spectroscopy (CRDS). Thus far, CRDS experiments have been performed using visible laser light at fixed standard wavelengths, such as 532 nm. However, since by far most compounds of analytical interest absorb in the ultraviolet (UV), it is of utmost importance to develop UV-CRDS. In this study, as a first step towards the deep-UV region, LC separations with CRDS detection (using a previously described liquid-only cavity flow cell) at 457 and 355 nm are reported for standard mixtures of dyes and nitro-polyaromatic hydrocarbons (nitro-PAHs), respectively. For the measurements in the blue range a home-built optical parametric oscillator (OPO) system, tunable between 425 and 478 nm, was used, achieving a baseline noise of 2.7 x 10(-6) A.U. at 457 nm, improving upon the sensitivity of conventional absorbance detection (typically around 10(-4) A.U.). An enhancement of the sensitivity can be seen at 355 nm as well, but the improvement of the baseline noise (1.3 x 10(-5) A.U.) is much less pronounced. The sensitivity at 355 nm is limited by the quality of the UV-CRDS mirrors that are currently available: whereas the ring-down times as obtained at 457 nm are around 70-80 ns for the eluent, they are only 20-25 ns at 355 nm. Critical laser characteristics for LC-CRDS measurements, such as pulse length and mode structure, are given and prospects for going to shorter wavelengths are discussed.

Journal Article↗

Assessing PAH exposure in feral finfish from the Northwest Atlantic.

Polycyclic aromatic hydrocarbon (PAH) concentrations were examined in small finfish (<30 cm) represented by capelin, sand lance, American plaice, yellowtail flounder and herring collected opportunistically in various NAFO divisions. Analyses were performed on whole fish and in a portion of the samples; concentrations in internal organs were compared to the rest of the carcass. The effect of pool size, size differences within and between species, lipid content and location were examined to interpret PAH concentrations. Measurements were carried out before the development of the Hibernia oil fields and represent baseline levels for future comparison. Limits in assessing future risk that could be due to discharges of produced water or accidental oil spills are also discussed. Increasing knowledge on the bioaccumulation of PAH, on the production of bile metabolites, the formation of DNA-adducts and of the potential toxic effects associated with PAH will lead to better ecosystem management and protection for future generations.

Animal Structures↗

Interfacing capillary electrophoresis and surface-enhanced resonance Raman spectroscopy for the determination of dye compounds.

The at-line coupling of capillary electrophoresis (CE) and surface-enhanced resonance Raman spectroscopy (SERRS) was optimized for the separation and subsequent spectroscopic identification of charged analytes (dye compounds). Raman spectra were recorded following deposition of the electropherogram onto a moving substrate. To this end a new interface was developed using a stainless steel needle as a (grounded) cathode. The outlet end of the CE capillary was inserted into this metal needle; CE buffer touching the needle tip served as the electrical connection for the CE separation. A translation table was used to move the TLC plate at a constant speed during the deposition. The distance between the tip of the fused silica column and the TLC plate was kept as small as possible in order to establish a constant bridge-flow, while avoiding direct contact. The dyes Basic Red 9 (BR9), Acid Orange 7 (AO7) and Food Yellow 3 (FY3) were used as test compounds. After CE separation in a 20 mM borate buffer at pH 10, after deposition, concentrated silver colloid was added to each analyte spot, followed by irradiation with 514.5 nm light from an argon ion laser to record the SERRS signal using a Raman microscope. Different types of silver colloids were tested: Lee-Meisel type (citrate), borate, and gold-coated silver. BR9 (positively charged) gave much more intense SERRS spectra than the two negatively charged dyes. For BR9 and AO7 the citrate-coated Lee-Meisel colloid yielded the most intense SERRS spectra. The CE-SERRS system was used to separate and detect the negatively charged dyes. Silver colloid and nitric acid (to improve adsorption) were added post-deposition. Even though their chemical structures are very similar, AO7 and FY3 could be readily distinguished based on their SERRS spectra. The limits of detection (S/N = 3) of the CE-SERRS system ranged from 6.7 x 10(-5) M (2.6 x 10(-12) mol injected) for FY3 down to 1.8 x 10(-6) M (7.0 x 10(-14) mol injected) for BR9.

Journal Article↗

Miniaturized cavity ring-down detection in a liquid flow cell.

A novel method for applying cavity ring-down spectroscopy in the liquid phase, compatible with LC analyses, is presented. The core of the setup is a home-built cavity ring-down flow cell (cell volume 12 microL) that is constructed using a silicon rubber spacer, which is clamped leak-tight between two high-reflectivity mirrors. The mirrors are in direct contact with the liquid flow, which provides for a small path length and short ring-down times. Inside the cavity there are no windows, reflection losses, or Brewster angles to be considered. Due to the small size of the presented cavity geometry, the setup can be implemented in conventional-size LC apparatuses. With a flow injection setup, a detection limit of 2.5 nM was obtained for Crystal Violet in ethanol, and the linear dynamic range of the system is at least 2 orders of magnitude. The method has the potential to become a powerful alternative for commercial LC UV/visible absorbance detectors.

Journal Article↗

Pyrene biotransformation and kinetics in the hepatopancreas of the isopod Porcellio scaber.

Various techniques exist for polycyclic aromatic hydrocarbon (PAH) determination in environmental samples, but an adequate risk assessment of PAHs should include aspects such as bioavailability of the contaminant and biotransformation capacity of the species under investigation. In this study, we provided an analysis of the kinetics of pyrene in the terrestrial isopod Porcellio scaber. Isopods were exposed to pyrene in their food (10 microg/g d/w) for 7 days followed by an elimination period of 7 days. The animals were dissected, and the hepatopancreases were analyzed for pyrene biotransformation products; nonmetabolised pyrene in the gut was also monitored. Concentrations of 1-hydroxypyrene in the hepatopancreas were very low. Almost all of the pyrene was found as three conjugates: pyrene-1-glucoside, pyrene-1-sulfate, and a third unknown 1-hydroxypyrene conjugate. Concentrations of the metabolites were extremely variable between individuals because of variable feeding activity. An apparent steady state was reached already after 24 hours of exposure, whereas elimination was complete 48 hours after ending the exposure. This rapid response to changes in the exposure concentration shows that terrestrial isopods have a high biotransformation capacity for PAHs. The data show that concentrations of parent PAHs will not provide a good indication of exposure in rapidly metabolizing invertebrates such as isopods; instead, pyrene metabolites may be considered a promising biomarker for bioavailability of PAH contamination in the field.

Animals↗

Environmental impact and recovery at two dumping sites for dredged material in the North Sea.

The environmental impact and recovery associated with the long and uninterrupted disposal of large volumes of moderately contaminated dredged material from the port of Rotterdam was studied at nearby dumping sites in the North Sea. Observations were made on sediment contamination, ecotoxicity, biomarker responses and benthic community changes shortly after dumping at the 'North' site had ceased and at the start of disposal at the new dumping site 'Northwest'. During the period of dumping, very few benthic invertebrates were found at the North site. Concentrations of cadmium, mercury, polychlorinated biphenyls (PCBs), polyaromatic hydrocarbons (PAHs) and tributyltin (TBT) in the fine sediment fraction (<63 microm) from this site were 2-3 times higher than at the reference site. In four different bioassays with marine invertebrates the sediments showed no acute toxic effects. In tissue (pyloric caeca) of resident starfish Asterias rubens, residual levels of mercury, zinc, PCBs and dioxin-like activity were never more than twice those at the reference site. Four different biomarkers (DNA integrity, cytochrome P450 content, benzo[a]pyrene hydroxylase activity and acetylcholinesterase inhibition) were used on the starfish tissues, but no significant differences were found between North and the reference site. Minor pathological effects were observed in resident dab Limanda limanda. One year after dumping had ceased at the North site, a significant increase in the species richness and abundance of benthic invertebrates and a concomitant decrease in the fine sediment fraction of the seabed were observed. After 8.2 million m3 of moderately contaminated dredged material had been dumped at the new dumping site Northwest, the species richness and abundance of benthic invertebrates declined over an area extending about 1-2 km eastwards. This correlated with a shift in sediment texture from sand to silt. The contamination of the fine sediment fraction at the Northwest location doubled. It is concluded that marine benthic resources at and around the dumping sites have been adversely affected by physical disturbance (burial, smothering). However, no causal link could be established with sediment-associated contaminants from the dredged spoils.

Animals↗

Sub-second liquid chromatographic separations by means of shear-driven chromatography.

Utilizing the concept of shear-driven chromatography, we have been able to realize reversed-phase LC separations in flat rectangular nano-channels coated with a C8 monolayer and being as thin as 100 nm. At this scale, the separation kinetics are strongly enhanced, as is witnessed by the extremely short time (< 0.1 s) needed to separate a mixture of coumarin dyes. The observed plate numbers are still relatively small, because the experiments were conducted in ultra-short columns (< or = 1 mm) and under injection band width-limiting conditions.

Chromatography, Liquid↗

Detection of nonderivatized peptides in capillary electrophoresis using quenched phosphorescence.

A capillary electrophoresis detection technique for (small) peptides is presented, i.e. quenched phosphorescence, a method that is generally applicable and does not require chemical derivatization. For this purpose, a novel phosphorophore, 1-bromo-4-naphthalenesulfonic acid (BrNS), was synthesized. BrNS has sufficient water solubility and provides strong phosphorescence at room temperature over a wide pH range. The detection is based on the dynamic quenching of the BrNS phosphorescence background signal by electron transfer from the amino group of the peptides at pH 9.5-10. For the di- and tripeptides Val-Tyr-Val, Val-Gly-Gly, Ala-Ser, Gly-Asn, Gly-Ala, and Gly-Tyr, detection limits in the range of 5-20 microg/L were obtained. The novel technique is even a good alternative for the (limited) group of peptides containing tyrosine and, thus, exhibiting native fluorescence as well as strong UV absorption: using Gly-Tyr, Val-Tyr-Val, methionine enkephalin, and human angiotensin II as test compounds, quenched phosphorescence detection was found to compare favorably with absorption detection at 190- and 266-nm laser-induced fluorescence detection, as performed with a recently developed, small-size, quadrupled Nd:YAG laser.

Angiotensin II↗

On-line identification method in column liquid chromatography: UV resonance Raman spectroscopy.

Ultraviolet resonance Raman spectroscopy (RRS) is presented as a novel identification tool for conventional-size column liquid chromatography (LC). The on-line coupling was made using a standard Z-shaped flow cell. A continuous-wave frequency-doubled argon ion laser operating at a wavelength of 244 nm was used for excitation. "On-the-fly" resonance Raman spectra of four model compounds, fluorene, phenanthrene, fluoranthene, and pyrene, were recorded after a standard acetonitrile/water reversed-phase LC separation. When applying a large-volume-injection procedure (32 mL), detection limits were at the nanogram per milliliter level. The results indicate that UV-RRS gives detailed spectral information at an appropriate sensitivity level so that coupling with LC becomes feasible.

Journal Article↗

Determination of isoflavone glucoside malonates in Trifolium pratense L. (red clover) extracts: quantification and stability studies.

Isoflavones, their glucosides and their glucoside malonates were determined in red clover leaf extracts using reversed-phase LC coupled to atmospheric pressure chemical ionisation mass spectrometry (APCI-MS), UV and fluorescence detectors and the stability of the malonates was investigated. Extracts can be stored at least 1-2 weeks at -20 degrees C without loss of malonates. In LC-separated fractions the malonates are most stable when stored at low temperature after evaporation to dryness. The concentrations of eight major isoflavones ranged from 0.04 to 5 mg/g leaves.

Atmospheric Pressure↗

UV-B absorbance and UV-B absorbing compounds (para-coumaric acid) in pollen and sporopollenin: the perspective to track historic UV-B levels.

UV-B absorbance and UV-B absorbing compounds (UACs) of the pollen of Vicia faba, Betula pendula, Helleborus foetidus and Pinus sylvestris were studied. Sequential extraction demonstrated considerable UV-B absorbance both in the soluble (acid methanol) and insoluble sporopollenin (acetolysis resistant residue) fractions of UACs, while the wall-bound fraction of UACs was small. The UV-B absorbance of the soluble and sporopollenin fraction of pollen of Vicia faba plants exposed to enhanced UV-B (10 kJ m(-2) day(-1) UV-B(BE)) was higher than that of plants that received 0 kJ m(-2) day(-1) UV-B(BB). Pyrolysis gas chromatography-mass spectrometry (py-GC-MS) analysis of pollen demonstrated that p-coumaric acid and ferulic acid formed part of the sporopollenin fraction of the pollen. The amount of these aromatic monomers in the sporopollenin of Vicia faba appeared to increase in response to enhanced UV-B (10 kJ m(-2) day(-1) UV-B(BE)). The detection limit of pyGC-MS was sufficiently low to quantify these phenolic acids in ten pollen grains of Betula and Pinus. The experimental data presented provide evidence for the possibility that polyphenolic compounds in pollen of plants are indicators of solar UV-B and may be applied as a new proxy for the reconstruction of historic variation in solar UV-B levels.

Coumaric Acids↗

Liquid-core waveguide technology for coupling column liquid chromatography and Raman spectroscopy.

The on-line coupling of liquid chromatography (LC) and Raman spectroscopy (RS) via an entirely plastic liquid-core waveguide (LCW) was optimized in terms of excitation wavelength of the laser, especially in relation to the fluorescence background, and the length of the LCW. Excitation at 632.8 nm (He-Ne laser) was found to be a good compromise between a wavelength long enough to strongly reduce the fluorescence background and, on the other hand, short enough to avoid (re)-absorption of laser light and Raman signals by H2O in LCWs of considerable length. This conclusion is supported by a theoretical discussion on the optimization of LCW lengths as function of the excitation wavelength for H2O and 2H2O. When using the He-Ne laser the optimum length is approximately 50 cm for H2O; this corresponds to a detection cell volume of 19 microl for an LCW of 220 microm I.D., which is fully compatible with conventional-size LC. The influence of an organic modifier, usually necessary for reversed-phase LC, on the free spectral window was evaluated. The potential applicability of LC-LCW-RS was shown for a mixture of adenosine 5'-monophosphate (AMP), guanosine 5'-monophosphate (GMP) and uridine 5'-monophosphate (UMP), utilizing an aqueous eluent without the addition of a modifier. Improved detectability was achieved by using the stopped-flow mode and applying a large-volume-injection procedure (injection volume: 200 microl). Under these conditions, the limit of identification for AMP, GMP and UMP was in the 0.1-0.5-mg/ml range.

Adenosine Monophosphate↗

Laser-induced fluorescence detection at 266 nm in capillary electrophoresis. Polycyclic aromatic hydrocarbon metabolites in biota.

The separation of five phenolic polycyclic aromatic hydrocarbon metabolites (hydroxy-PAHs) has been performed by cyclodextrin-modified micellar electrokinetic chromatography (CD-MEKC) using a 30 mM borate buffer (pH 9.0) containing 60 mM sodium dodecyl sulfate and varying concentrations of gamma-cyclodextrin (gamma-CD). A concentration of 12.5 mM gamma-CD was found to provide a baseline separation of the five hydroxy-PAHs. We applied conventional fluorescence and laser-induced fluorescence (LIF) detection, using a new, small-size, quadrupled Nd-YAG laser emitting at 266 nm. The best limits of detection, in the low ng/ml range, were achieved using LIF detection. For all analytes, linearity was observed up to ca. 100 ng/ml. As an application, conjugated pyrene metabolites in hepatopancreas samples from the terrestrial isopods Oniscus asellus and Porcellio scaber were separated and detected. Finally, flatfish bile samples from individuals exposed to polluted sediment or crude oil, which were part of an interlaboratory study, were analyzed by CD-MEKC with conventional fluorescence and LIF detection to determine the 1-hydroxypyrene concentrations.

Animals↗

Applicability of surface-enhanced resonance Raman scattering for the direct discrimination of ballpoint pen inks.

In situ surface-enhanced resonance Raman spectroscopy (SERRS) with excitation at 685 nm is suitable for the direct discrimination of blue and black ballpoint pen inks on paper. For black inks, shorter excitation wavelengths can also be used. For blue inks, SERRS at 514.5 and 457.9 nm does not provide adequate discriminative power. At these excitation wavelengths, the SERRS signals of the Methyl Violet derivatives present in inks easily dominate the overall spectrum because of resonance enhancement and preferential interaction with silver sol particles. At 685 nm, this problem is not encountered as the Methyl Violet derivatives do not show resonance enhancement, while other components may still exhibit resonance. Thirteen blue and thirteen black ink lines were examined. For the blue and black inks, on the basis of the 685 nm SERR spectra, eight and six groups of spectra, respectively, could be distinguished. This discrimination largely agrees with information from thin layer chromatography (TLC) experiments, although some differences in group compositions are found. The in situ SERR spectra show good repeatability with regard to the Raman frequencies, band shapes and relative intensities of the spectral bands. However, absolute intensities cannot be used for discrimination purposes.

Journal Article↗

Organic contaminants and trace metals in flounder liver and sediment from the Amsterdam and Rotterdam harbours and off the Dutch coast.

Organic contaminants [polychlorinated biphenyls (PCBs), organochlorine pesticides (OCPs), polybrominated diphenylethers (PBDEs), nonylphenols], organotin compounds and trace metals (cadmium, chromium, mercury and zinc) were determined in flounder (Platichthys flesus) liver and sediment from the Amsterdam harbour (North Sea Canal) and Rotterdam harbour (Euromonding) and off the Dutch coast between the Amsterdam and Rotterdam harbour mouths in order to assess the level of contamination in these harbours and to study contamination gradients.

Animals↗

Dose- and time-dependent formation of biliary benzo[a]pyrene metabolites in the marine flatfish dab (Limanda limanda).

Polycyclic aromatic hydrocarbons (PAHs) are abundant pollutants, and many PAHs are carcinogenic, but only after metabolic activation. Benzo[a]pyrene (BaP) is among the most carcinogenic PAHs. The dose and time response of two enzymes involved in BaP metabolism and the amounts of BaP metabolites excreted into the bile were evaluated in an experiment with dab (Limanda limanda). Ninety dab were exposed orally to one of five doses of BaP (0, 0.08, 0.4, 2, or 10 mg/kg) and sampled at 3, 6, or 12 d after exposure. None of the doses studied caused significant induction of either microsomal ethoxyresorufin-O-deethylase (EROD). which reflects cytochrome P450 1A (CYP1A) activity, or cytosolic glutathione-S-transferase activity (GST). Concentrations of biliary BaP metabolites significantly increased with dose and significantly decreased with time after exposure. It is concluded that biliary BaP metabolites provide a much more sensitive method than EROD (CYP1A) or GST activity to monitor recent exposure to PAHs in dab.

Administration, Oral↗

Surface-enhanced resonance Raman spectroscopy as an identification tool in column liquid chromatography.

The compatibility of ion-pair reversed-phase column liquid chromatography and surface-enhanced resonance Raman spectroscopy (SERRS) for separation and identification of anionic dyes has been investigated, with emphasis on the at-line coupling via a thin-layer chromatography (TLC) plate. SERR spectra using silver sols were recorded both for aqueous solutions and for samples deposited on aluminum oxide and silica TLC plates at 514.5- and 457.9-nm laser excitation. For some dyes, the shorter wavelength was needed to diminish the fluorescence background. For aqueous solutions and for samples deposited on aluminum oxide, clear SERR spectra were obtained upon addition of poly(L-lysine); for the silica plates, the addition of nitric acid was required. Upon drying the plates, the SERRS signals decreased in intensity; simply adding a drop of water could largely restore them. At-line coupling of LC and SERRS was successfully achieved when using silica, but not aluminum oxide, plates. The application of a gradient, a high water content, and the presence of ion-pair reagents needed for the separation did not adversely affect the deposition and the recording of SERR spectra. The identification limits were 10-20 ng of deposited material, depending on the dye selected, which corresponded to injected concentrations of 5-10 microg mL(-1).

Journal Article↗

Preparation, isolation, and characterization of Dibenzo[a,l]pyrene diol epoxide-deoxyribonucleoside monophosphate adducts by HPLC and fluorescence line-narrowing spectroscopy.

Dibenzo[a,l]pyrene (DB[a,l]P) is the most potent carcinogenic polycyclic aromatic hydrocarbon that has been identified in the environment. Earlier studies in our laboratory indicated that more than 80% of the DB[a,l]P-DNA adducts formed in vitro were depurinating adducts and that most of the stable adducts were formed from diol epoxide intermediates. To complete the profile of both stable and depurinating adducts of DB[a,l]P, we have synthesized standard adducts by reacting 3'-dAMP or 3'-dGMP with either (+/-)-anti- or (+/-)-syn-dibenzo[a,l]pyrene 11,12-dihydrodiol 13, 14-epoxide (DB[a,l]PDE). The adducts were separated by HPLC with an ion-pair column and were identified by fluorescence line-narrowing spectroscopy (FLNS). A total of six pairs of stereoisomers along with another stable DB[a,l]PDE-DNA adduct were successfully isolated and identified. Pairs of (+/-)-trans and (+/-)-cis isomers were expected to be formed from the reaction of anti-DB[a,l]PDE with either dAMP or dGMP. While we were able to identify two pairs of stereoisomeric (+/-)-syn-DB[a,l]PDE-dAMP (cis and trans) and two pairs of stereoisomeric (+/-)-anti-DB[a,l]PDE-dAMP (cis and trans) adducts, identification of all the stereoisomers of dGMP adducts proved to be impossible. A pair of (+/-)-syn-trans-DB[a,l]PDE-dGMP adducts, a pair of (+/-)-anti-cis-DB[a,l]PDE-dGMP adducts, and one syn-cis-DB[a,l]PDE-dGMP adduct were conclusively identified by FLNS. These standard adducts will be used to identify the stable DNA adducts formed by DB[a,l]P and DB[a,l]PDE in vitro and in vivo.

Benzopyrenes↗