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PubMed2004

Uses of speciation techniques in biomonitoring for assessing human exposure to organic environmental chemicals.

Speciation analysis has been used for many years to identify and measure different forms of a given chemical in environmental and human samples. Although the term "speciation" is generally applied to the measurement of inorganic chemicals, the term can also be applied to many measurements of organic chemicals in complex samples, such as environmental media and biological matrices. We present several examples of achieving speciation analysis by selecting the appropriate biological matrix in which to measure a specific chemical(s), by a given analytical method, for the most accurate assessment of human exposure to the environmental chemical. Much of this information and many of these techniques are transferable to the measurement of inorganic elements in environmental and biological samples.

Environmental Exposure↗

PubMed2001

Analytical methodologies for aluminium speciation in environmental and biological samples--a review.

It is recognized that aluminium (Al) is a potential environmental hazard. Acidic deposition has been linked to increased Al concentrations in natural waters. Elevated levels of Al might have serious consequences for biological communities. Of particular interest is the speciation of Al in aquatic environments, because Al toxicity depends on its forms and concentrations. In this paper, advances in analytical methodologies for Al speciation in environmental and biological samples during the past five years are reviewed. Concerns about the specific problems of Al speciation and highlights of some important methods are elucidated in sections devoted to hybrid techniques (HPLC or FPLC coupled with ET-AAS, ICP-AES, or ICP-MS), flow-injection analysis (FIA), nuclear magnetic resonance (27Al NMR), electrochemical analysis, and computer simulation. More than 130 references are cited.

Aluminum↗

PubMed2001

Coupling pervaporation to AAS for inorganic and organic mercury determination. A new approach to speciation of Hg in environmental samples.

The design and development of a new approach for Hg speciation in environmental samples is described in detail. This method, consisting of the coupling of pervaporation and atomic absorption spectrometry, is based on a membrane phenomenon that combines the evaporation of volatile analytes and their diffusion through a polymeric membrane. It is proposed here as an alternative to gas chromatography for speciation of inorganic and organic Hg compounds, as the latter compounds are volatile and can be separated by applying the principles mentioned above. The interest of this method lies in its easy handling, low cost, and rapidity for the analysis of liquid and solid samples. This method has been applied to Hg speciation in a compost sample provided by a waste water treatment plant.

Calibration↗

PubMed1995

Speciation of Se, Fe and Zn in Human Milk Whey: The use of Instrumental Neutron Activation Analysis (INAA) to corroborate element profiles measured with Inductively Coupled Plasma Atomic Emission Spectrometry (ICP-AES).

In human milk trace elements normally exist in a form which can easily be absorbed by the newborn infant. For investigations of the bioavailability of trace elements it is necessary to carry out a speciation analysis of the elements of interest. An independent analytical method has been used for the quality control of the shape of the element profiles obtained from the speciation analysis of Se, Fe and Zn in individual samples of human milk whey after chromatographic separation. For the element detection in the untreated milk fractions Instrumental Neutron Activation Analysis (INAA) was chosen as the reference method. Element distribution patterns have been obtained with Inductively Coupled Plasma Atomic Emission Spectrometry (ICP-AES) using on-line digestion of the fraction, reduction and hydride formation of Se ("T"-mode). Prior results are compared with those obtained by means of element detection in the untreated fractions ("U"-mode) with ICP-AES. The elution profiles of Se, Fe and Zn in human milk whey obtained by means of ICP-AES detection using the "T"-mode show good agreement with the distribution patterns obtained with INAA. Recoveries of 103% for Fe, 86% for Zn and 87% for Se were obtained. The element distribution patterns of Fe and Zn obtained with ICP-AES speciation using the "T"-mode also show good agreement with those obtained by means of ICP-AES using the "U"-mode.

Journal Article↗

PubMed1996

Speciation of mercury, platinum and tin - focus of research and future developments.

A discussion about the elements mercury, platinum and tin and their organometallic compounds, with special attention to important aspects like anthropogenic emissions, use in industry, agriculture and medicine, toxicities, biogeochemical cycles, highlights the necessity of speciation analysis. Methods frequently used to speciate mercury, platinum and tin compounds in different matrices are summarized. Future trends are indicated in order to give an impression about the importance of metal speciation and its increasing impact on some key disciplines.

Journal Article↗

PubMed1996

Soil bacteria sensitivity towards heavy metals - Experimental system optimisation using chemical speciation calculations.

The ecotoxicological relevance of many laboratory studies on soil bacteria sensitivity towards heavy metals is limited because culture conditions are chosen which do not adequately represent field conditions. The influence of the composition of culture media on the speciation of copper in an oligotrophic model soil system has been investigated. The expected chemical speciation has been calculated to obtain information on the concentration of the bioavailable fraction and the totally dissolved copper. For control measurements of totally dissolved copper, vacuum filtration has been used. The results of the measurements are in a good agreement with the calculations. Therefore, the use of speciation calculations is postulated as a useful tool for the assessment of free metal concentrations at higher pH, where the concentrations of dissolved metals are too low to be measured by simple methods.

Journal Article↗

PubMed1996

Atomic absorption spectrometry (AAS) - a versatile and selective detector for trace element speciation.

AAS as a highly sensitive and specific single element technique is ideally suited as a detector for speciation analysis. The combinations of chromatographic separation with element specific detectors (flame AAS, electrothermal AAS (ETAAS), hydride generation AAS (HGAAS)) provide powerful approaches to the determination of all species. Sample stabilisation is the area that requires most attention as it still represents the main source of problems encountered in speciation work. The correct speciation depends on how the sample is handled prior to analysis. Unfortunately, no universal procedure has been found. Anything that changes redox conditions, pH or complexation equilibrium is clearly unacceptable.

Journal Article↗

PubMed2002

Copper speciation and accumulation in the gill microenvironment of carp ( Cyprinus carpio) in the presence of kaolin particles.

Carp were exposed to copper adsorbed on kaolin particles at various concentrations (0-2.4 mg/L), and net accumulation due to elevated adsorbed copper in the surrounding water was observed. Copper speciation in the water and fish gill microenvironment was modeled in the presence and absence of kaolin using a chemical speciation program (MINTEQA2). The adsorption affinity constants of kaolin for copper at various pH values used in the speciation calculations were experimentally determined, and the quantitative relationship between the affinity constant and pH was modeled. Copper accumulations in fish gills exposed to kaolin-adsorbed copper was then observed. The results indicate that desorption occurred in the fish gill microenvironment due to both mucus competition of copper and slight increase in water pH. Furthermore, the available copper species increased as a result of desorption, causing a net accumulation of Cu by the gills.

Adsorption↗

PubMed2004

Principal biogeochemical factors affecting the speciation and transport of mercury through the terrestrial environment.

It is increasingly becoming known that mercury transport and speciation in the terrestrial environment play major roles in methyl-mercury bioaccumulation potential in surface water. This review discusses the principal biogeochemical reactions affecting the transport and speciation of mercury in the terrestrial watershed. The issues presented are mercury-ligand formation, mercury adsorption/desorption, and elemental mercury reduction and volatilization. In terrestrial environments, OH-, Cl- and S- ions have the largest influence on ligand formation. Under oxidized surface soil conditions Hg(OH)2, HgCl2, HgOH+, HgS, and Hg0 are the predominant inorganic mercury forms. In reduced environments, common mercury forms are HgSH+, HgOHSH, and HgClSH. Many of these mercury forms are further bound to organic and inorganic ligands. Mercury adsorption to mineral and organic surfaces is mainly dictated by two factors: pH and dissolved ions. An increase in Cl- concentration and a decrease in pH can, together or separately, decrease mercury adsorption. Clay and organic soils have the highest capability of adsorbing mercury. Important parameters that increase abiotic inorganic mercury reduction are availability of electron donors, low redox potential, and sunlight intensity. Primary factors that increase volatilization are soil permeability and temperature. A decrease in mercury adsorption and an increase in soil moisture will also increase volatilization. The effect of climate on biogeochemical reactions in the terrestrial watershed indicates mercury speciation and transport to receiving water will vary on a regional basis.

Adsorption↗

PubMed2005

Arsenic speciation analysis in water samples: a review of the hyphenated techniques.

Interests in the determination of different arsenic species in natural waters is caused by the fact that toxic effects of arsenic are connected with its chemical forms and oxidation states. In determinations of water samples inorganic arsenate (As(III), As(V)), methylated metabolities (MMAA, DMAA) and other organic forms such as AsB, AsC, arsenosugars or arsenic containing lipids have the most importance. This article provides information about occurrence of the dominant arsenic forms in various water environments. The main factors controlling arsenic speciation in water are described. The quantification of species is difficult because the concentrations of different forms in water samples are relatively low compared to the detection limits of the available analytical techniques. Several hyphenated methods used in arsenic speciation analysis are described. Specific advantages and disadvantages of methods can define their application for a particular sample analysis. Insufficient selectivity and sensitivity of arsenic speciation methods cause searching for a new or modifications already existing techniques. Some aspects of improvement and modifications of the methods are highlighted.

Arsenates↗

PubMed1993

Speciation patterns of ectoparasites and "straggling" lice.

Two competing views have been expressed to explain ectoparasite speciation patterns, one emphasizing co-speciation and one emphasizing host-switching. Though recent authors preferred a combination of these views, the available phylogenetic trees cannot be interpreted without revisiting island biogeography theory. Parasite extinction due to a temporal decline in host population size seems to be a prerequisite of subsequent speciation by host-switch. The need for a re-evaluation of "stragglers" (ectoparasites found on non-specific hosts) is emphasized.

Animals↗

PubMed1989

Inorganic chemistry of chromium and its speciation in Whetlerite.

Chromium compounds are among the impregnants that enhance the ability of carbon air filters to absorb and destroy toxic agents such as CK and AC. The possibility of inhaling chromium-containing carbon dust from such filters has caused concern because, in addition to being an essential nutrient, chromium has been identified as a chemical carcinogen in humans. The essentiality or carcinogenicity of chromium depends upon its chemical speciation. Solubility and oxidation state are particularly important factors in assessing the potential hazards associated with the possible inhalation of chromium-containing dusts from these impregnated carbons or Whetlerites. The chemical speciation of the chromium in Whetlerite was found to be: from 0.6 to 1.3% insoluble trivalent chromium; from 1.0 to 1.3% insoluble hexavalent chromium; and from 0.7 to 0.9% soluble hexavalent chromium. The impregnation process, and the resulting speciation of chromium in Whetlerite, is consistent with the inorganic chemistry of chromium.

Air Pollutants, Occupational↗

PubMed1989

Speciation and bifurcations.

The interrelations of physics and biology are discussed. It is shown that Darwin can be considered as one of the founders of the important field of contemporary physics called physics of dissipative structures or synergetics. The theories of gradual and punctual evolution are presented. The contradiction between these theories can be solved on the basis of molecular theory of evolution and on the basis of the phenomenological physical treatment. The general physical properties of living systems, considered as open systems being far from equilibrium, are listed and simple non-linear mathematical models describing gradual and punctual speciation are suggested. The usual pictures which present these two kinds of speciation can possess physico-mathematical sense. Punctuated speciation means bifurcation, a kind of non-equilibrium phase transition.

Biological Evolution↗

PubMed2006

Imaging and speciation of trace elements in biological environment.

Mineral elements, often at the trace level, play a considerable role in physiology and pathology of biological systems. Metallogenomics, metalloproteomics, and metallomics are among the emerging disciplines which are critically dependent on spatially resolved concentration maps of trace elements in a cell or tissue, on information on chemical speciation, and on that on metal-binding coordination sites. The mini-review discusses recent progress in analytical techniques for element profiling on the genome scale, biological trace element imaging, and probing, identification and quantification of chemical species in the biological environment. Imaging of the element distribution in cells and tissue sections is becoming possible with sub-micrometer spatial resolution and picogram-level sensitivity owing to advances in laser ablation MS, ion beam and synchrotron radiation X-ray fluorescence microprobes. Progress in nanoflow chromatography and capillary electrophoresis coupled with element specific ICP MS and molecule-specific electrospray MS/MS and MALDI enables speciation of elements in microsamples in a complex biological environment. Laser ablation ICP MS, micro-SXRF, and micro-PIXE allow mapping of trace element distribution in 1D and 2D proteomics gels. The increasing sensitivity of EXAFS and XANES owing to the use of more intense synchrotron beams and efficient focusing optics provide information about oxidation state, fingerprint speciation of metal sites and metal-site structures.

Environmental Pollution↗

PubMed2006

Diel cycles of arsenic speciation due to photooxidation in acid mine drainage from the Iberian Pyrite Belt (Sw Spain).

Twenty four hours diel cycles of arsenic speciation in Acid Mine Drainage (AMD) due to photooxidation have been reported for the first time. AMD samples were taken during 48 h (31st March and 1st April, 2005) at 6 h intervals from the effluent of a massive abandoned polymetallic sulphide mine of the Iberian Pyrite Belt (Sw Spain). Samples were preserved in situ using cationic exchange prior to analysis by coupled high performance liquid chromatography, hydride generation and atomic fluorescence spectrometry (HPLC-HG-AFS) for arsenic speciation. The results indicated the presence of inorganic arsenic species with daily means of 262mugl(-1) for As(V) and 107 microg l(-1) for As(III). No marked diel trend was observed for As(V). However, a marked diel trend was observed for As(III) in the two studied days, with maximum concentrations during nighttime (141-143 microg l(-1)) and minimum concentrations at daytime (72-77 microg l(-1)). This difference in concentration during daytime and nighttime is ca. 100%. A similar diel cycle was observed for iron. An explanation for the arsenic diel cycles observed is the light induced photooxidation of As(III) and the elimination of As(V) due to its adsorption onto Fe precipitates during the daytime. Furthermore, the diel changes in arsenic speciation emphasize the importance of designing suitable sampling strategies in AMD systems.

Arsenic↗

PubMed2006

Arsenic speciation of atmospheric particulate matter (PM10) in an industrialised urban site in southwestern Spain.

An arsenic speciation study has been performed in PM10 samples collected on a fortnight basis in the city of Huelva (SW Spain) during 2001 and 2002. The arsenic species were extracted from the PM10 filters using a NH2OH x HCl solution and sonication, and determined by HPLC-HG-AFS. The mean bulk As concentration of the samples analyzed during 2001 and 2002 slightly exceed the mean annual 6 ng m(-3) target value proposed by the European Commission for 2013, arsenate [As(V)] being responsible for the high level of arsenic. The speciation analyses showed that As(V) was the main arsenic species found, followed by arsenite [As(III)] (mean 6.5 and 7.8 ng m(-3) for As(V), mean 1.2 and 2.1 ng m(-3) for As(III), in 2001 and 2002, respectively). The high levels of arsenic species found in PM10 in Huelva have a predominant industrial origin, such as the one from a nearby copper smelter, and do not present a seasonal pattern. The highest daily levels of arsenic species correspond to synoptic conditions in which the winds with S and SW components transport the contaminants from the main emission source. The frequent African dust outbreaks over Huelva may result in an increment of mass levels of PM10, but do not represent a significant input of arsenic in comparison to the anthropogenic source. The rural background levels of arsenic around Huelva are rather high, in comparison to other rural or urban areas in Spain, showing a relatively high atmosphere residence time of arsenic. This work shows the importance of arsenic speciation in studies of aerosol chemistry, due to the presence of arsenic species [As(III) and As(V)] with distinct toxicity.

Air Pollutants↗

PubMed2006

Evolution of heavy metal speciation during the aerobic composting process of sewage sludge.

The contents of heavy metals and their bioavailability to the soil-plant system were the major limitation to the application of sewage sludge compost in soil. This study was conducted to determine the evolution of heavy metal speciation in the course of an aerobic composting, and investigate the influence of changes of composting process parameters including pH, temperature and organic matter (OM) content on distribution of heavy metal speciation in composted sludge. The sequential extraction procedure developed by Tessier et al. was used in sludge compost to determine the heavy metal speciation. Results showed that, during composting, (1) the contents of the residue fraction for Pb, Zn and Cd were decreased but those for Ni and Cr were increased; the Cu residue fraction was almost constant; (2) the contents of the total mobile fractions (including fractions 1-4) for Zn and Pb were significantly increased, but the increase of those for Cu and Ni were not so remarkable; (3) there were significant degrees of correlation between heavy metal fractions and changes of some selected parameters (for example, pH, composting temperature, and OM content). Only the content of the total mobile fractions for Cu could be predictable from its total content. For the prediction of the total mobile fractions of Zn, Ni, Cd and Cr, the R(2) value was significantly increased by the inclusion of other variables such as pH, temperature and OM content.

Aerobiosis↗

PubMed2006

A review of total dissolved copper and its chemical speciation in San Francisco Bay, California.

Following basin-wide contamination from industrial emissions and urban development, total dissolved copper concentrations in some regions of San Francisco Bay have exceeded national and state guidelines for water quality. In the face of dramatic improvements in wastewater treatment and point source control, persisting elevated dissolved copper concentrations in the Bay have prompted multiple studies and extensive monitoring of this estuary since 1989. Statistical analyses of monitoring data show that total dissolved copper concentrations have declined in the North (by 17%) and South (29%) San Francisco Bay as well as in the Southern Sloughs (44%) from 1993 to 2001. Concentrations remain elevated in the farthest reaches of the Bay (Delta and Estuary Interface), and in the Central Bay. Dissolved copper concentrations throughout the Bay have also been positively correlated (r = 0.632, P < 0.0005, n = 598) with dissolved organic matter, supporting results from complimentary chemical speciation studies which indicate that high-affinity copper-binding organic ligands dominate the chemical speciation of dissolved copper in the Bay. These organic ligands typically bind > 99.9% of the dissolved copper, effectively buffering the system against small changes in dissolved copper concentrations, and maintaining free Cu(2+) concentrations well below the toxicity threshold of ambient aquatic microorganisms. In response to these findings, site-specific water quality criteria for dissolved copper concentrations are now being developed by the Regional Water Quality Board to provide a more appropriate standard for copper toxicity in the Bay-one based on its chemical speciation and bioavailability.

Biological Availability↗