Theoretical models of mercury dissolution from dental amalgams in neutral and acidic flows

R. G. Keanini, Jack Ferracane, T. Okabe

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

This article reports an experimental and theoretical investigation of mercury dissolution from dental amalgams immersed in neutral (noncorrosive) and acidic (corrosive) flows. Atomic absorption spectrophotometric measurements of Hg loss indicate that in neutral flow, surface oxide films formed in air prior to immersion persist and effectively suppress significant mercury release. In acidic (pH 1) flows, by contrast, oxide films are unstable and dissolve; depending on the amalgam's material composition, particularly its copper content, two distinct mercury release mechanisms are initiated. In low copper amalgam, high initial mercury release rates are observed and appear to reflect preferential mercury dissolution from unstable Sn8Hg (γ2) grains within the amalgam matrix. In high copper amalgam, mercury release rates are initially low, but increase with time. Microscopic examination suggests that this feature reflects corrosion of copper from grains of Cu6Sn5 (η′) and consequent exposure of Ag2Hg31) grains; the latter serve as internal mercury release sites and become more numerous as corrosion proceeds. Three theoretical models are proposed in order to explain observed dissolution characteristics. Model I, applicable to high and low copper amalgams in neutral flow, assumes that mercury dissolution is mediated by solid diffusion within the amalgam, and that a thin oxide film persists on the amalgam's surface and lumps diffusive in-film transport into an effective convective boundary condition. Model II, applicable to low copper amalgam in acidic flow, assumes that the amalgam's external oxide film dissolves on a short time scale relative to the experimental observation period; it neglects corrosive suppression of mercury transport. Model III, applicable to high copper amalgam in acidic flow, assumes that internal mercury release sites are created by corrosion of copper in η′ grains and that corrosion proceeds via an oxidation-reduction reaction involving bound copper and diffusing hydrogen ions. The models appear to capture the correct time dependence of each dissolution mechanism and to provide reasonable fits to the experimental data.

Original languageEnglish (US)
Pages (from-to)409-416
Number of pages8
JournalMetallurgical and Materials Transactions B: Process Metallurgy and Materials Processing Science
Volume32
Issue number3
StatePublished - Jun 2001

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Dental amalgams
Dental Amalgam
Mercury amalgams
Mercury (metal)
Mercury
Dissolution
Copper
Oxide films
Corrosion
Caustics
Diffusion in solids
Redox reactions
Protons
Microscopic examination

ASJC Scopus subject areas

  • Materials Science(all)
  • Metals and Alloys

Cite this

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title = "Theoretical models of mercury dissolution from dental amalgams in neutral and acidic flows",
abstract = "This article reports an experimental and theoretical investigation of mercury dissolution from dental amalgams immersed in neutral (noncorrosive) and acidic (corrosive) flows. Atomic absorption spectrophotometric measurements of Hg loss indicate that in neutral flow, surface oxide films formed in air prior to immersion persist and effectively suppress significant mercury release. In acidic (pH 1) flows, by contrast, oxide films are unstable and dissolve; depending on the amalgam's material composition, particularly its copper content, two distinct mercury release mechanisms are initiated. In low copper amalgam, high initial mercury release rates are observed and appear to reflect preferential mercury dissolution from unstable Sn8Hg (γ2) grains within the amalgam matrix. In high copper amalgam, mercury release rates are initially low, but increase with time. Microscopic examination suggests that this feature reflects corrosion of copper from grains of Cu6Sn5 (η′) and consequent exposure of Ag2Hg3 (γ1) grains; the latter serve as internal mercury release sites and become more numerous as corrosion proceeds. Three theoretical models are proposed in order to explain observed dissolution characteristics. Model I, applicable to high and low copper amalgams in neutral flow, assumes that mercury dissolution is mediated by solid diffusion within the amalgam, and that a thin oxide film persists on the amalgam's surface and lumps diffusive in-film transport into an effective convective boundary condition. Model II, applicable to low copper amalgam in acidic flow, assumes that the amalgam's external oxide film dissolves on a short time scale relative to the experimental observation period; it neglects corrosive suppression of mercury transport. Model III, applicable to high copper amalgam in acidic flow, assumes that internal mercury release sites are created by corrosion of copper in η′ grains and that corrosion proceeds via an oxidation-reduction reaction involving bound copper and diffusing hydrogen ions. The models appear to capture the correct time dependence of each dissolution mechanism and to provide reasonable fits to the experimental data.",
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AU - Ferracane, Jack

AU - Okabe, T.

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N2 - This article reports an experimental and theoretical investigation of mercury dissolution from dental amalgams immersed in neutral (noncorrosive) and acidic (corrosive) flows. Atomic absorption spectrophotometric measurements of Hg loss indicate that in neutral flow, surface oxide films formed in air prior to immersion persist and effectively suppress significant mercury release. In acidic (pH 1) flows, by contrast, oxide films are unstable and dissolve; depending on the amalgam's material composition, particularly its copper content, two distinct mercury release mechanisms are initiated. In low copper amalgam, high initial mercury release rates are observed and appear to reflect preferential mercury dissolution from unstable Sn8Hg (γ2) grains within the amalgam matrix. In high copper amalgam, mercury release rates are initially low, but increase with time. Microscopic examination suggests that this feature reflects corrosion of copper from grains of Cu6Sn5 (η′) and consequent exposure of Ag2Hg3 (γ1) grains; the latter serve as internal mercury release sites and become more numerous as corrosion proceeds. Three theoretical models are proposed in order to explain observed dissolution characteristics. Model I, applicable to high and low copper amalgams in neutral flow, assumes that mercury dissolution is mediated by solid diffusion within the amalgam, and that a thin oxide film persists on the amalgam's surface and lumps diffusive in-film transport into an effective convective boundary condition. Model II, applicable to low copper amalgam in acidic flow, assumes that the amalgam's external oxide film dissolves on a short time scale relative to the experimental observation period; it neglects corrosive suppression of mercury transport. Model III, applicable to high copper amalgam in acidic flow, assumes that internal mercury release sites are created by corrosion of copper in η′ grains and that corrosion proceeds via an oxidation-reduction reaction involving bound copper and diffusing hydrogen ions. The models appear to capture the correct time dependence of each dissolution mechanism and to provide reasonable fits to the experimental data.

AB - This article reports an experimental and theoretical investigation of mercury dissolution from dental amalgams immersed in neutral (noncorrosive) and acidic (corrosive) flows. Atomic absorption spectrophotometric measurements of Hg loss indicate that in neutral flow, surface oxide films formed in air prior to immersion persist and effectively suppress significant mercury release. In acidic (pH 1) flows, by contrast, oxide films are unstable and dissolve; depending on the amalgam's material composition, particularly its copper content, two distinct mercury release mechanisms are initiated. In low copper amalgam, high initial mercury release rates are observed and appear to reflect preferential mercury dissolution from unstable Sn8Hg (γ2) grains within the amalgam matrix. In high copper amalgam, mercury release rates are initially low, but increase with time. Microscopic examination suggests that this feature reflects corrosion of copper from grains of Cu6Sn5 (η′) and consequent exposure of Ag2Hg3 (γ1) grains; the latter serve as internal mercury release sites and become more numerous as corrosion proceeds. Three theoretical models are proposed in order to explain observed dissolution characteristics. Model I, applicable to high and low copper amalgams in neutral flow, assumes that mercury dissolution is mediated by solid diffusion within the amalgam, and that a thin oxide film persists on the amalgam's surface and lumps diffusive in-film transport into an effective convective boundary condition. Model II, applicable to low copper amalgam in acidic flow, assumes that the amalgam's external oxide film dissolves on a short time scale relative to the experimental observation period; it neglects corrosive suppression of mercury transport. Model III, applicable to high copper amalgam in acidic flow, assumes that internal mercury release sites are created by corrosion of copper in η′ grains and that corrosion proceeds via an oxidation-reduction reaction involving bound copper and diffusing hydrogen ions. The models appear to capture the correct time dependence of each dissolution mechanism and to provide reasonable fits to the experimental data.

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