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Particles, sweat, and tears: A comparative study on bioaccessibility of ferrochromium alloy and stainless steel particles, the pure metals and their metal oxides, in simulated skin and eye contact
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.ORCID iD: 0000-0003-2145-3650
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.ORCID iD: 0000-0003-2206-0082
2010 (English)In: Integrated Environmental Assessment and Management, ISSN 1551-3793, ISSN 1551-3793, Vol. 6, no 3, 456-468 p.Article in journal (Refereed) Published
Abstract [en]

Ferrochromium alloys are manufactured in large quantities and placed on the global market for use as master alloys (secondary raw materials), primarily for stainless steel production. Any potential human exposure to ferrochromium alloy particles is related to occupational activities during production and use, with 2 main exposure routes, dermal contact and inhalation and subsequent digestion. Alloy and reference particles exposed in vitro in synthetic biological fluids relevant for these main exposure routes have been investigated in a large research effort combining bioaccessibility; chemical speciation; and material, surface, and particle characteristics. In this paper, data for the dermal exposure route, including skin and eye contact, will be presented and discussed. Bioaccessibility data have been generated for particles of a ferrochromium alloy, stainless steel grade AISI 316L, pure Fe, pure Cr, iron(II,III)oxide, and chromium(III)oxide, upon immersion in artificial sweat (pH 6.5) and artificial tear (pH 8.0) fluids for various time periods. Measured released amounts of Fe, Cr, and Ni are presented in terms of average Fe and Cr release rates and amounts released per amount of particles loaded. The results are discussed in relation to bulk and surface composition of the particles. Additional information, essential to assess the bioavailability of Cr released, was generated by determining its chemical speciation and by providing information on its complexation and oxidation states in both media investigated. The effect of differences in experimental temperature, 30 °C and 37 °C, on the extent of metal release in artificial sweat is demonstrated. Iron was the preferentially released element in all test media and for all time periods and ironcontaining particles investigated. The extent of metal release was highly pH dependent and was also dependent on the medium composition. Released amounts of Cr and Fe were very low (close to the limit of detection, <0.008% of particles released or dissolved as iron or chromium) for the alloy particles (ferrochromium alloy and stainless steel), the pure Cr particles, and the metal oxide particles. The released fraction of Cr (Cr/[Cr + Fe]) varied with the material investigated, the test medium, and the exposure time and cannot be predicted from either the bulk or the surface composition. Chromium was released as noncomplexed Cr(III) and in addition in very low concentrations (<3 mg/L). Nickel released was under the limit of detection (0.5 mg/L), except for ultrafine stainless steel particles (<10 mg/L). It is evident that media chemistry and material properties from a bulk and surface perspective, as well as other particle characteristics, and the chemical speciation of released metals have to be considered when assessing any potential hazard or risk induced by sparingly soluble metal or alloy particles.

Place, publisher, year, edition, pages
2010. Vol. 6, no 3, 456-468 p.
Keyword [en]
Bioaccessibility, Chemical speciation, Dermal contact, Ferrochromium alloy, Metal particles
National Category
Physical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-14307DOI: 10.1002/ieam.66PubMedID: 20821707Scopus ID: 2-s2.0-77954692674OAI: oai:DiVA.org:kth-14307DiVA: diva2:332174
Note

QC 20100803

Available from: 2010-08-03 Created: 2010-08-03 Last updated: 2014-04-11Bibliographically approved
In thesis
1. Metal Particles – Hazard or Risk? Elaboration and Implementation of a Research Strategy from a Surface and Corrosion Perspective
Open this publication in new window or tab >>Metal Particles – Hazard or Risk? Elaboration and Implementation of a Research Strategy from a Surface and Corrosion Perspective
2009 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Do metal particles (including particles of pure metals, alloys, metal oxides and compounds) pose a hazard or risk to human health? In the light of this question, this thesis summarizes results from research conducted on metal particles, and describes the elaboration and implementation of an in vitro test methodology to study metal release from particles through corrosion and dissolution processes in synthetic biological media relevant for human exposure through inhalation/ingestion and dermal contact.

Bioaccessible metals are defined as the pool of released metals from particles that potentially could be made available for absorption by humans or other organisms. Studies of bioaccessible metals from different metal particles within this thesis have shown that the metal release process is influenced by material properties, particle specific properties, size distribution, surface area and morphology, as well as the chemistry of synthetic biological test media simulating various human exposure scenarios. The presence of metal particles in proximity to humans and the fact that metals can be released from particles to a varying extent is the hazard referred to in the title.

The bioavailable metal fraction of the released metals (the fraction available for uptake/absorption by humans through different exposure routes) is usually significantly smaller than the bioaccessible pool of released metals, and is largely related to the chemical form and state of oxidation of the released metals. Chemical speciation measurements of released chromium for instance revealed chromium to be complexed to its non-available form in simulated lung fluids. Such measurements provide an indirect measure of the potential risk for adverse health effects, when performed at relevant experimental conditions.

A more direct way to assess risks is to conduct toxicological in-vitro testing of metal particles, for instance on lung cell cultures relevant for human inhalation. Induced toxicity of metal particles on lung cells includes both the effect of the particles themselves and of the released metal fraction (including bioaccessible and bioavailable metals), the latter shown to be less predominant. The toxic response was clearly influenced by various experimental conditions such as sonication treatment of particles and the presence of serum proteins.

Thorough characterization of metal particles assessing parameters including chemical surface composition, degree of agglomeration in solution, size distribution, surface area and morphology was performed and discussed in relation to generated results of bioaccessibility, bioavailability and induced toxicity. One important conclusion was that neither the surface composition nor the bulk composition can be used to assess the extent of metals released from chromium-based alloy particles. These findings emphasize that information on physical-chemical properties and surface characteristics of particles is essential for an in-depth understanding of metal release processes and for further use and interpretation of bioaccessibility data to assess hazard and reduce any risks induced by human exposure to metal particles.

Place, publisher, year, edition, pages
Stockholm: KTH, 2009. xiv, 69 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2009:56
Keyword
ferro-chromium alloy, metal particles, bioaccessibility, chemical speciation, dermal contact, surface oxide, in-vitro testing, chemical speciation, cu, copper, comet assay, intracellular, ultrafine, in vitro, A549, cytotoxicity, DNA damage, nanoparticles, particle characterization, artificial sweat, nickel release, nickel powder particles, particle loadings, release kinetics, surface area, copper release, powder particles, synthetic body fluids, simulation of interstitial lung conditions, skin contact, metal release, stainless steel, particles, test method
National Category
Physical Chemistry Analytical Chemistry Analytical Chemistry
Identifiers
urn:nbn:se:kth:diva-11695 (URN)978-91-7415-472-6 (ISBN)
Public defence
2009-12-14, F3, Lindstedtsvägen 26, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Note
QC 20100803Available from: 2009-12-04 Created: 2009-12-03 Last updated: 2010-08-03Bibliographically approved
2. Environmental and health aspects of corrosion– importance of chemical speciation
Open this publication in new window or tab >>Environmental and health aspects of corrosion– importance of chemical speciation
2010 (English)Licentiate thesis, comprehensive summary (Other academic)
Abstract [en]

During the last decades, the interest in corrosion of metals and alloys from an environmental and health perspective has increased rapidly as a consequence of stricter environmental and human exposure legislations, their extensive use as implant materials and an increasing understanding related to occupational and/or daily exposure to airborne particles. Corrosion-induced metal release, however, needs to be understood in detail and to include knowledge related to chemical speciation, i.e. the oxidation state, complexation and chemical form of released metals, parameters of high importance when considering toxicity.

In this licentiate work, corrosion-induced metal runoff from roofing materials (copper, zinc, and chromium(III)-, and chromium(VI) surface treated galvanized steel) has been investigated from an environmental perspective with focus on chemical speciation of released metals (Papers I-II). From these papers it was evident that the total concentration measured in the runoff water is not sufficient for any environmental risk assessment. The environmental fate including changes in chemical speciation and hence metal precipitation has to be considered. For example, it was shown that the copper concentration decreased by three orders of magnitude already in the internal drainage system of a shopping centre with a copper roof, to a concentration lower than storm water collected from a nearby parking space (Paper I). Also, speciation measurements can explain corrosion, metal release and surface processes of chromium surface treated galvanized steel at different sites (urban and marine). Any environmental risk assessment has to be done by considering all metal species released, and compared with ecotoxic values. For example, when most chromium(VI) (the most toxic species) was released, significantly less zinc was released at the same time which decreased the overall ecotoxicity of the runoff water significantly (Paper II).

When assessing environmental risks by standard laboratory tests, it is important to understand all mechanisms which are possibly influenced by individual experimental parameters and which often are different for different test substances. Some metals released, as seen in the case of iron, may precipitate with time and be pH-, solution- and buffering dependent. This behavior can lead to strongly underestimated measured metal concentrations (Paper III).

When particles of metals or alloys are to be investigated (Papers III-VI), it is essential to conduct a thorough particle characterization, since the surface properties cannot be defined. In addition, the surface properties (oxide layer properties) change with varying particle size (Paper VI) and with other experimental parameters such as dispersion (Paper VI).

All iron-, and chromium-based particles investigated (Papers III-VI) revealed large differences between alloy particles and pure metals. Particles of pure iron and nickel released significantly more metals compared with particles of the investigated alloys, whereas particles of pure chromium released less metals compared with the alloys. Particles of stainless steel (AISI 316L), ferro-chromium and ferro-silicon-chromium released very low amounts of metals (Papers III-VI). The released quantity increased with increased acidity (Papers III-VI) and also in the presence of complexing agents (ongoing research). The manufacturing process is of high importance, as observed for stainless steel particles when compared with a side product from stainless steel production with similar composition that released significantly more metals (Paper III). Particles of metal oxides, i.e. chromium(III)oxide and iron(II,III)oxide, released very low amounts of metals due to their thermodynamic stability.

Ongoing research activities focus on the specific influence of complexing agents and proteins on the metal release process from massive sheet and particles of metals and alloys. The applicability and the possibility to use different analytical tools are investigated and elaborated for small-sized particles. A detailed understanding of the correlation between material and particle characteristics, the metal release process, the chemical speciation in interaction with proteins and/or cells, and the particle/cell interaction is essential to enable any correlation between material/particle characteristics and toxicity.

The aim of this licentiate summary is – in contrast to the six included scientific papers – to explain the importance of chemical speciation for corrosion processes from a health and environmental perspective in a popular way to reach a broad non-academic audience. The summary is hence written as a guidance document for stakeholders and the regulatory community working with environmental and health risk assessment.

Place, publisher, year, edition, pages
Stockholm, Sweden: KTH, 2010. xvi, 36 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 32
Identifiers
urn:nbn:se:kth:diva-24701 (URN)978-91-7415-716-1 (ISBN)
Presentation
2010-10-28, conference room 3, YKI, Drottning Kristinas väg 49A, Stockholm, 10:00 (English)
Opponent
Supervisors
Note
QC 20101006Available from: 2010-10-06 Created: 2010-09-23 Last updated: 2010-12-14Bibliographically approved

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Hedberg, YolandaOdnevall Wallinder, Inger

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