PubMed Health⌕ Search

Biomedical subjects

Manuel Miró

Publications and source records attributed to Manuel Miró.

14 recordsLinked to original sources

Hyphenating multisyringe flow injection lab-on-valve analysis with atomic fluorescence spectrometry for on-line bead injection preconcentration and determination of trace levels of hydride-forming elements in environmental samples.

In this work the third generation of flow injection analysis, that is, the so-called micro-lab-on-valve (microLOV) approach, is proposed for the first time for the separation, preconcentration, and monitoring of metalloids as hyphenated with atomic fluorescence spectrometry (AFS). This was made feasible by interfacing the micromachined LOV-module with AFS by a multisyringe flowing stream network for on-line postcolumn derivatization of the eluate aimed at generation of hydride species. The potential of this new hyphenated technique for environmental assays was ascertained via determination of ultratrace level concentrations of total inorganic arsenic in freshwater. Employing quantitative preoxidation of As(III) to As(V) in the samples by means of permanganate, the method involves preconcentration of arsenate at pH 10 on a renewable anion exchanger, namely, Q-Sepharose, packed in a LOV microcolumn. The analyte species is afterward stripped out and concurrently prereduced by a 300 microL eluent plug containing 6 mol L(-)1 HCl and 10% KI. The eluate is downstream merged with a metered volume of sodium tetrahydroborate (0.3% w/v) for generation of arsine, which is subsequently quantified by AFS. The flow system facilitates on-column reduction of the retained arsenic with no need for application of programmable stopped flow. Yet, the high concentration of reductant and extreme pH conditions for elution hinder the sorbent to be reused due to gradual deactivation of the functional moieties, so that maximum benefit can be taken from the application of the bead renewable strategy. The proposed procedure is characterized by a high tolerance to metal species and interfering hydride-forming elements. In fact, ratios of Se(IV) to As < or = 5000 and Sb(V) to As < or = 500 are tolerated at the 10% interference level. Under the optimized experimental conditions, a detection limit (3sigma) of 0.02 ng mL(-1) As, a dynamic linear range of 0.05-2.0 ng mL(-1) As (by tailoring the AFS gain), an enrichment factor of 8.8 for arsenate, and a precision better than 6.0% at the 0.1 ng mL-1 level were obtained for the bead-injection mode whenever the loading sample volume was affixed at 3.0 mL. The reliability and accuracy of the automated procedure was ascertained by determining total inorganic arsenic in both spiked environmental waters and certified reference materials of variable matrix complexity (TMDA-54.3 and ERM-CA010) at the low ng mL(-1) level. No significant differences were found between the experimental results and the certified values at a significance level of 0.05.

Journal Article↗

Development of a simple extraction cell with bi-directional continuous flow coupled on-line to ICP-MS for assessment of elemental associations in solid samples.

A continuous-flow system comprising a novel, custom-built extraction module and hyphenated with inductively coupled plasma-mass spectrometric (ICP-MS) detection is proposed for assessing metal mobilities and geochemical associations in soil compartments as based on using the three step BCR (now the Measurements and Testing Programme of the European Commission) sequential extraction scheme. Employing a peristaltic pump as liquid driver, alternate directional flows of the extractants are used to overcome compression of the solid particles within the extraction unit to ensure a steady partitioning flow rate and thus to maintain constant operationally defined extraction conditions. The proposed flow set-up is proven to allow for trouble-free handling of soil samples up to 1 g and flow rates < or =10 mL min(-1). The miniaturized extraction system was coupled to ICP-MS through a flow injection interface in order to discretely introduce appropriate extract volumes to the detector at a given time and with a given dilution factor. The proposed hyphenated method demonstrates excellent performance for on-line monitoring of major and trace elements (Ca, Mn, Fe, Ni, Pb, Zn and Cd) released when applying the various extracting reagents as addressed in the BCR scheme, that is, 0.11 M CH(3)COOH, 0.1 NH(2)OH.HCl and 30% H(2)O(2), even when a well recognized matrix-sensitive detector, such as ICP-MS, is used. As a result of the enhanced temporal resolution of the ongoing extraction, insights into the breaking down of phases and into the kinetics of the metal release are obtained. With the simultaneous multielement detection capability of ICP-MS, the dynamic fractionation system presents itself as an efficient front-end for evaluation of actual elemental association by interelement comparison of metals leached concurrently during the extraction time. Thus, the intimate elemental association between Cd and Zn in contaminated soils could be assessed.

Chemical Fractionation↗

Highly selective micro-sequential injection lab-on-valve (muSI-LOV) method for the determination of ultra-trace concentrations of nickel in saline matrices using detection by electrothermal atomic absorption spectrometry.

A highly selective procedure is proposed for the determination of ultra-trace level concentrations of nickel in saline aqueous matrices exploiting a micro-sequential injection Lab-On-Valve (muSI-LOV) sample pretreatment protocol comprising bead injection separation/pre-concentration and detection by electrothermal atomic absorption spectrometry (ETAAS). Based on the dimethylglyoxime (DMG) reaction used for nickel analysis, the sample, as contained in a pH 9.0 buffer, is, after on-line merging with the chelating reagent, transported to a reaction coil attached to one of the external ports of the LOV to assure sufficient reaction time for the formation of Ni(DMG)(2) chelate. The non-ionic coordination compound is then collected in a renewable micro-column packed with a reversed-phase copolymeric sorbent [namely, poly(divinylbenzene-co-N-vinylpyrrolidone)] containing a balanced ratio of hydrophilic and lipophilic monomers. Following elution by a 50-muL methanol plug in an air-segmented modality, the nickel is finally quantified by ETAAS. Under the optimized conditions and for a sample volume of 1.8 mL, a retention efficiency of 70 % and an enrichment factor of 25 were obtained. The proposed methodology showed a high tolerance to the commonly encountered alkaline earth matrix elements in environmental waters, that is, calcium and magnesium, and was successfully applied for the determination of nickel in an NIST standard reference material (NIST 1640-Trace elements in natural water), household tap water of high hardness and local seawater. Satisfying recoveries were achieved for all spiked environmental water samples with maximum deviations of 6 %. The experimental results for the standard reference material were not statistically different to the certified value at a significance level of 0.05.

Journal Article↗

Automated on-line renewable solid-phase extraction-liquid chromatography exploiting multisyringe flow injection-bead injection lab-on-valve analysis.

In this paper, the third generation of flow injection analysis, also named the lab-on-valve (LOV) approach, is proposed for the first time as a front end to high-performance liquid chromatography (HPLC) for on-line solid-phase extraction (SPE) sample processing by exploiting the bead injection (BI) concept. The proposed microanalytical system based on discontinuous programmable flow features automated packing (and withdrawal after single use) of a small amount of sorbent (<5 mg) into the microconduits of the flow network and quantitative elution of sorbed species into a narrow band (150 microL of 95% MeOH). The hyphenation of multisyringe flow injection analysis (MSFIA) with BI-LOV prior to HPLC analysis is utilized for on-line postextraction treatment to ensure chemical compatibility between the eluate medium and the initial HPLC gradient conditions. This circumvents the band-broadening effect commonly observed in conventional on-line SPE-based sample processors due to the low eluting strength of the mobile phase. The potential of the novel MSFI-BI-LOV hyphenation for on-line handling of complex environmental and biological samples prior to reversed-phase chromatographic separations was assessed for the expeditious determination of five acidic pharmaceutical residues (viz., ketoprofen, naproxen, bezafibrate, diclofenac, and ibuprofen) and one metabolite (viz., salicylic acid) in surface water, urban wastewater, and urine. To this end, the copolymeric divinylbenzene-co-n-vinylpyrrolidone beads (Oasis HLB) were utilized as renewable sorptive entities in the micromachined unit. The automated analytical method features relative recovery percentages of >88%, limits of detection within the range 0.02-0.67 ng mL(-1), and coefficients of variation <11% for the column renewable mode and gives rise to a drastic reduction in operation costs ( approximately 25-fold) as compared to on-line column switching systems.

Automation↗

On-line dynamic extraction and automated determination of readily bioavailable hexavalent chromium in solid substrates using micro-sequential injection bead-injection lab-on-valve hyphenated with electrothermal atomic absorption spectrometry.

A novel and miniaturized micro-sequential injection bead-injection lab-on-valve (microSI-BI-LOV) fractionation system was developed for on-line microcolumn soil extraction under simulated environmental scenarios and accurate monitoring of the content of easily mobilisable hexavalent chromium in soil environments at the sub-low parts-per-million level. The flow system integrates dynamic leaching of hexavalent chromium using deionized water as recommended by the German Standard DIN 38414-S4 method; on-line pH adjustment of the extract by a 0.01 mol L(-1) Tris-HNO(3) buffer solution; isolation of the chromate leached from the matrix constituents onto a Q Sepharose strong anion-exchanger freshly packed into the microconduits of the microSI-assembly; air-segmented elution of the sorbed species by a 40 microL plug of 0.5 mol L(-1) NH(4)NO(3) (pH 8) eluent; and detection by electrothermal atomic absorption spectrometry (ETAAS). The effect of simulated acidic rain on the accessibility of chromate forms for plant uptake was also investigated. The proposed approach offers several advantages over conventional speciation/fractionation protocols in the batch mode, including immediate separation with concomitant preconcentration of the released chromate, minimization of Cr(vi) to Cr(iii) interconversion risks, enhanced accuracy, and non-existence of re-adsorption/re-distribution problems along with a detailed pattern of the kinetics of the leaching process. The reliability of the proposed method was evaluated via spiking of a moderately polluted agricultural soil material (San Joaquin Soil-Baseline Trace Element Concentrations) with water-soluble Cr(vi) salts at different concentration levels. The potential of the microSI-BI-LOV set-up with renewable surfaces for flame-AAS determination of high levels of readily bioavailable chromate in contaminated soils is also addressed.

Biological Availability↗

Universal approach for selective trace metal determinations via sequential injection-bead injection-lab-on-valve using renewable hydrophobic bead surfaces as reagent carriers.

A new concept is presented for selective and sensitive determination of trace metals via electrothermal atomic absorption spectrometry based on the principle of bead injection (BI) with renewable reversed-phase surfaces in a sequential injection-lab-on-valve (SI-LOV) mode. The methodology involves the use of poly(styrene-divinylbenzene) beads containing pendant octadecyl moieties (C18-PS/DVB), which are preimpregnated with a selective organic metal chelating agent prior to the automatic manipulation of the beads in the microbore conduits of the LOV unit. By adapting this approach, the immobilization of the most suitable chelating agent can be effected irrespective of the kinetics involved, optimal reaction conditions can be used for implementing the chelating reaction of the target metal analyte with the immobilized re-agent, and an added degree of freedom is offered in selecting the most favorable elution mode in order to attain the highest sensitivity. The potential of the SI-BI-LOV scheme is demonstrated by taking Cr(VI) as a model analyte, using a 1,5-diphenylcarbazide (DPC)-loaded bead column as the active microzone. As this reaction requires the use of high acidity, it is also shown that the bead material exhibits excellent chemical stability at low pH values. On-line pH sample adjustment prevents alteration of the original distribution of chromium species while ensuring fast rates for the DPC-Cr(VI) reaction. The proposed procedure was successfully applied to the determination of trace levels of Cr(VI) in natural waters containing high levels of dissolved salts (such as seawater and hard tap water) without requiring any dilution step. Method validation was performed by determination of total chromium in an NIST standard reference material (NIST 1640, natural water) after Cr(III) oxidation, and the results were in good agreement with the certified value.

Journal Article↗

Automated sequential injection-microcolumn approach with on-line flame atomic absorption spectrometric detection for implementing metal fractionation schemes of homogeneous and nonhomogeneous solid samples of environmental interest.

An automated sequential injection (SI) system incorporating a dual-conical microcolumn is proposed as a versatile approach for the accommodation of both single and sequential extraction schemes for metal fractionation of solid samples of environmental concern. Coupled to flame atomic absorption spectrometric detection and used for the determination of Cu as a model analyte, the potentials of this novel hyphenated approach are demonstrated by the ability of handling up to a 300 mg sample of a nonhomogeneous sewage amended soil (viz., CRM 483). The three steps of the endorsed Standards, Measurements, and Testing sequential extraction method have been also performed in a dynamic fashion and critically compared with the conventional batchwise protocols. The ecotoxicological relevance of the data provided by both methods with different operationally defined conditions is thoroughly discussed. As compared to traditional batch systems, the developed SI assembly offers minimal risks of sample contamination, the absence of metal re-distribution/readsorption, and dramatic saving of operational times (from 16 h to 40-80 min per partitioning step). It readily facilitates the accurate manipulation of the extracting reagents into the flow network and the minute, well-defined injection of the desired leachate volume into the detector. Moreover, highly time-resolved information on the ongoing extraction is given, which is particularly relevant for monitoring fast leaching kinetics, such as those involving strong chelating agents. On-line and off-line (for Cu, Pb, and Zn) single extraction schemes are also proven to constitute attractive alternatives for fast screening of metal pollution in solid samples and for predicting the current, rather than the potential, element bioavailability by the assessment of the readily mobilizable metal forms.

Journal Article↗

A novel dynamic approach for automatic microsampling and continuous monitoring of metal ion release from soils exploiting a dedicated flow-through microdialyser.

In this paper, a novel concept is presented for automatic microsampling and continuous monitoring of metal ions in soils with minimum disturbance of the sampling site. It involves a hollow-fiber microdialyser that is implanted in the soil body as a miniaturized sensing device. The idea behind microdialysis in this application is to mimic the function of a passive sampler to predict the actual, rather than potential, mobility and bioavailability of metal traces. Although almost quantitative dialysis recoveries were obtained for lead (> or = 98%) from aqueous model solutions with sufficiently long capillaries (l > or = 30 mm, 200 microm i.d.) at perfusion rates of 2.0 microL min(-1), the resistance of an inert soil matrix was found to reduce metal uptake by 30%. Preliminary investigation of the potential of the microdialysis analyser for risk assessment of soil pollution, and for metal partitioning studies, were performed by implanting the dedicated probe in a laboratory-made soil column and hyphenating it with electrothermal atomic absorption spectrometry (ETAAS), so that minute, well-defined volumes of clean microdialysates were injected on-line into the graphite furnace. A noteworthy feature of the implanted microdialysis-based device is the capability to follow the kinetics of metal release under simulated natural scenarios or anthropogenic actions. An ancillary flow set-up was arranged in such a way that a continuous flow of leaching solution--mild extractant (10(-2) mol L(-1) CaCl2), acidic solution (10(-3) mol L(-1) HNO3), or chelating agent (10(-4) or 10(-2) mol L(-1) EDTA)--was maintained through the soil body, while the concentration trends of inorganic (un-bound) metal species at the soil-liquid interface could be monitored at near real-time. Hence, relevant qualitative and quantitative information about the various mobile fractions is obtained, and metal-soil phase associations can also be elucidated. Finally, stimulus-response schemes adapted from neurochemical applications and pharmacokinetic studies are to be extended to soil research as an alternative means of local monitoring of extraction processes after induction of a chemical change in the outer boundary of the permselective dialysis membrane.

Journal Article↗

Flow-through optical fiber sensor for automatic sulfide determination in waters by multisyringe flow injection analysis using solid-phase reflectometry.

A software-controlled flow-through optical fiber diffuse reflectance sensor capitalized on the implementation of disk-based solid-phase pre-concentration schemes in a multisyringe flow injection analysis (MSFIA) set-up is proposed for the trace determination of sulfide in environmental waters and wastewaters. The fully automated flowing methodology is based on Fischer's coupling reaction of sulfide with N,N-dimethyl-p-phenylenediamine (DMPD) in the presence of Fe(iii) as oxidizing reagent in a 0.5 M HCl medium. The on-line generated methylene blue dye is subsequently delivered downstream to a dedicated optode cell furnished with an octadecyl-chemically modified (C(18)) disk, while continuously recording the diffuse reflectance spectrum of the pre-concentrated compound. A double regeneration protocol is finally executed to warrant minimum background noise and negligible baseline. Under the optimized chemical and hydrodynamic conditions, the optosensing MSFIA method features coefficients of variation better than 0.7%(n= 10) at 50 microg l(-1) concentration, a linear working range of 20-200 microg l(-1) sulfide, a 3sigma(blank) detection limit of 2.9 microg l(-1) sulfide and an injection throughput of 8 h(-1) for a pre-concentration sample volume of 2.9 ml. The interfacing of the robust and versatile multisyringe flow injection-based optode with a plug-in spectrophotometer furnished with a light emitting diode assures the miniaturization of the overall flow analyzer, which is, thus, readily adaptable to real-time monitoring schemes. The potential of the multisyringe flow method was assessed via the determination of sulfide traces in water samples of different complexity (namely, freshwater, seawater and wastewater).

Fiber Optic Technology↗

Implantable flow-through capillary-type microdialyzers for continuous in situ monitoring of environmentally relevant parameters.

In this paper, a simple, flexible, and cost-effective flow-through microdialyzer hyphenated with a miniaturized differential potentiometric detector is proposed for continuous diffusion-controlled sampling of analytes of environmental interest. The analytical performance of the dedicated configuration involving merely a single cellulose regenerated hollow fiber is critically compared with that of commercially available concentric probes commonly exploited for in vivo monitoring of the extracellular space in living tissues and that of large dialysis-based probes furnished with flat membranes. The outstanding feature of the capillary-type design is the ability of adapting the extraction fractions (EF) to the requirements of the assays and flow-through detectors by selection of appropriate membrane length/perfusion rate ratios. Passive sampling under steady-state conditions (EF approximately 100%) has proven feasible for environmentally relevant ions, such as chloride, by perfusing a 3-cm-long capillary with water at a flow rate of 2.0 microL/min. Hence, there is no need for recalibration of the flow setup after implantation of the purpose-made probe. The effect of physical and chemical variables on the diffusive flux is discussed in detail for the various flow-through membrane separation devices assessed. Effective means to attain identical dialysate concentrations of target species under dynamic regime irrespective of the matrix ingredients are also presented. The dedicated microdialyzer features extreme tolerance to high molecular weight interfering matrix compounds (> or =5000 mg/L humic acid) at the 5% interference level, which makes it especially suited for the interference-free potentiometric determination of ionic species in environmental samples containing high levels of organic matter. The potentials of the membrane separation unit were assessed for continuous monitoring of chemical changes in the interstitial/pore water of organic soils via stimulus-response strategies.

Chlorides↗

Automated enzymatic assays in a renewable fashion using the multisyringe flow injection scheme with soluble enzymes.

In this paper, a novel flowing stream scheme based upon the multisyringe flow injection (MSFI) technique is presented as a powerful tool to perform automated enzymatic assays. The exploitation of enzymes in homogeneous phase circumvents typical drawbacks associated with the commonly used packed-bead or open tubular permanent columns, namely, malfunctions of the reactor, carryover effects, flow resistance, loss of binding sites, large reagent consumption, and use of harmful organic solvents during immobilization procedures. The proposed MSFI system is able to handle minute volumes of soluble enzymes and accommodate reactions with divergent kinetic and pH demands, as demonstrated via the indirect chemiluminescence determination of trace levels of glucose. The procedure is based on the on-line glucose oxidase-catalyzed oxidation of beta-glucose in homogeneous phase to beta-glucono-delta-lactone and hydrogen peroxide. Subsequently, the generated oxidant merges downstream with an alkaline slug of 3-aminopthalhydrazide and a metal-catalyst zone (viz., Co(II)) at a total flow rate as high as 72 mL/min aiming to warrant maximum light collection from the fast CL reaction. Under optimum conditions for both sequentially occurring reactions, a glucose concentration as low as 90 microg/L may be easily detected at a 1000-fold photomultiplier gain. A second-order polynomial regression equation of light emission versus substrate concentration is found over the range 90 microg/L-2.7 mg/L glucose, although a maximum concentration of 180 mg/L may be determined by suitable gain selection without requiring manifold reconfiguration. An injection throughput of 20 h(-1), a repeatability better than 2.5% at the 1 mg/L level, and a 3sigma detection limit of 72 microg/L are the analytical features of the designed analyzer. The proposed approach was applied to the analysis of ultralow glucose content soft drinks as well as fruit juices suitable for diabetic consumers. The accuracy was assessed using the spectrophotometric batch glucose-Trinder method as an external reference methodology for the determination of the target species in parenteral solutions.

Catalysis↗

A novel flow-through microdialysis separation unit with integrated differential potentiometric detection for the determination of chloride in soil samples.

In this paper, a novel and miniaturised flow-through dialysis-based potentiometric detector is proposed for the determination of chloride in soil samples. The outstanding feature of the designed unit is the integration of analyte isolation from matrix constituents via membrane separation with differential potentiometric detection. Two identical tubular all-solid-state Ag/AgCl ion selective electrodes (ISEs) were assembled respectively at the inlet and outlet of the acceptor channel. Thus, as a consequence of the continuous forward flow of solutions through the microdialyser the outlet tube becomes the indicator electrode for the analyte diffusate while the nested tube at the entrance serves as reference electrode. The effect of physical and chemical parameters on the mass transfer efficiency is discussed in detail and compared with conventional configurations involving downstream detection. The membrane morphology for optimum dialysis performance is also thoroughly evaluated in terms of thickness, porosity and molecular weight cut-off. Higher dialysis efficiency and reduction of dilution factors up to a value of 5 were attained by halting the recipient stream temporarily. Under the optimised conditions, a dynamic working range of 5-5000 mg l(-1) chloride with a linear interval between 10 and 5000 mg l(-1) (for 1 min stopped-flow and 200 microl sample volume), a repeatability better than 3.0% and a 3 sigma(blank) detection limit of 1.2 mg l(-1) chloride were the analytical figures of merit of the devised configuration. The potentiometric dialysis sensor features extreme tolerance to high molecular weight interfering matrix compounds (> 1000 mg l(-1) humic acid), which makes it specially suited for the interference-free potentiometric determination of chloride in soils containing high levels of organic matter. The miniature size, low-reagent consumption and high analytical throughput (25-40 h(-1)) also warrant its applicability to in-field monitoring or screening schemes. The accuracy of the measurements was assessed using ion-chromatography as an external reference method. A mean t-test showed no statistical differences between both methodologies at the 95% confidence level.

Chlorides↗

Sequential injection 90Sr determination in environmental samples using a wetting-film extraction method.

A sequential injection procedure involving a flow-reversal wetting-film extraction method for the determination of the radionuclide 90Sr has been developed. The methodology is based on the coating of the inner walls of an open tubular reactor with a film prepared from a 0.14 M 4,4'(5')-bis(tert-butylcyclohexano)-18-crown-6 (BCHC) solution in 1-octanol, which allows the selective isolation of strontium from the sample matrix. Selection of the optimum extractant diluent attending its physical properties, investigation of the extraction kinetics features, and choice of the proper elution procedure are discussed in detail in this paper. The noteworthy aspects of using a wetting-film phase instead of a solid-phase material described to date in the literature are the reduction of crown ether consumption and the simplification of both the operational sequence and the automation of the extractant-phase renewal between consecutive samples, which is of interest to avoid analyte carryover and reduction of the resin capacity factor caused by irreversible interferences. The proposed method has been successfully applied to different spiked environmental samples (water, milk, and soil), with 90Sr total activities ranging between 0.07 and 0.30 Bq, measured using a low-background proportional counter. The standard deviation of the automated analytical separation procedure is lower than 3% (n = 10), and the 90Sr isolation process under the studied conditions may be carried out with a yield up to 80%.

Algorithms↗