Oxidative dissolution of metacinnabar (β-HgS) by dissolved oxygen
Identifieur interne : 010C34 ( Main/Repository ); précédent : 010C33; suivant : 010C35Oxidative dissolution of metacinnabar (β-HgS) by dissolved oxygen
Auteurs : RBID : Pascal:01-0485812Descripteurs français
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Abstract
The oxidative dissolution rate of metacinnabar by dissolved O2 was measured at pH ∼5 in batch and column reactors. In the batch reactors, the dissolution rate varied from 3.15 (±0.40) to 5.87 (±0.39) × 10-2 μmol/m2/day (I = 0.01 M, 23°C) and increased with stirring speed, a characteristic normally associated with a transport-controlled reaction. However, theoretical calculations, a measured activation energy of 77 (±8) kJ/mol (I = 0.01 M), and the mineral dis-solution literature indicate reaction rates this slow are unlikely to be transport controlled. This phenomenon was attributed to the tendency of the hydrophobic source powder to aggregate and minimize the effective outer surface area. However, in a column experiment, the steady-state dissolution rate ranged from 1.34 (±0.11) to 2.27 (±0.11)x 10-2 μmol/m2/day (I = 0.01 M, 23°C) and was also influenced by flow rate, suggesting hydrodynamic conditions may influence weathering rates observed in the field. The rate of Hg release to solution, under a range of hydrogeochemical conditions that more closely approximated those in the subsurface, was 1 to 3 orders of magnitude lower than the conditions that more closely approximated those in the subsurface, was 1 to 3 orders of magnitude lower than the dissolution rate due to the adsorption of released Hg(II) to the metacinnabar surface. The measured dissolution rates under all conditions were slow compared to the dissolution rates of minerals typically considered stable in the environment, and the adsorption of Hg(II) to the metacinnabar surface further lowered the Hg release rate.
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<record><TEI><teiHeader><fileDesc><titleStmt><title xml:lang="en" level="a">Oxidative dissolution of metacinnabar (β-HgS) by dissolved oxygen</title>
<author><name sortKey="Barnett, Mark O" uniqKey="Barnett M">Mark O. Barnett</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>Environmental Sciences Division, Oak Ridge National Laboratory Oak Ridge</s1>
<s2>TN, 37831-6038</s2>
<s3>USA</s3>
<sZ>1 aut.</sZ>
<sZ>2 aut.</sZ>
</inist:fA14>
<country>États-Unis</country>
<placeName><region type="state">Tennessee</region>
</placeName>
</affiliation>
<affiliation wicri:level="1"><inist:fA14 i1="02"><s1>Environmental Sciences and Engineering, University of North Carolina</s1>
<s2>Chapel Hill, NC, 27599-7400</s2>
<s3>USA</s3>
<sZ>1 aut.</sZ>
<sZ>3 aut.</sZ>
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<country>États-Unis</country>
<wicri:noRegion>Chapel Hill, NC, 27599-7400</wicri:noRegion>
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</author>
<author><name sortKey="Turner, Ralph R" uniqKey="Turner R">Ralph R. Turner</name>
<affiliation wicri:level="1"><inist:fA14 i1="01"><s1>Environmental Sciences Division, Oak Ridge National Laboratory Oak Ridge</s1>
<s2>TN, 37831-6038</s2>
<s3>USA</s3>
<sZ>1 aut.</sZ>
<sZ>2 aut.</sZ>
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<country>États-Unis</country>
<placeName><region type="state">Tennessee</region>
</placeName>
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<author><name sortKey="Singer, Philip C" uniqKey="Singer P">Philip C. Singer</name>
<affiliation wicri:level="1"><inist:fA14 i1="02"><s1>Environmental Sciences and Engineering, University of North Carolina</s1>
<s2>Chapel Hill, NC, 27599-7400</s2>
<s3>USA</s3>
<sZ>1 aut.</sZ>
<sZ>3 aut.</sZ>
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<country>États-Unis</country>
<wicri:noRegion>Chapel Hill, NC, 27599-7400</wicri:noRegion>
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<publicationStmt><idno type="inist">01-0485812</idno>
<date when="2001">2001</date>
<idno type="stanalyst">PASCAL 01-0485812 INIST</idno>
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<seriesStmt><idno type="ISSN">0883-2927</idno>
<title level="j" type="abbreviated">Appl. geochem.</title>
<title level="j" type="main">Applied geochemistry</title>
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</fileDesc>
<profileDesc><textClass><keywords scheme="KwdEn" xml:lang="en"><term>adsorption</term>
<term>astatine</term>
<term>beryllium</term>
<term>carbon</term>
<term>dissolution</term>
<term>experimental studies</term>
<term>hydrochemistry</term>
<term>hydrodynamics</term>
<term>indium</term>
<term>iodine</term>
<term>mercury</term>
<term>metacinnabar</term>
<term>oxygen</term>
<term>pH</term>
<term>solution rates</term>
<term>sulfides</term>
<term>surface water</term>
<term>transport</term>
<term>weathering</term>
</keywords>
<keywords scheme="Pascal" xml:lang="fr"><term>Sulfure</term>
<term>Metacinabre</term>
<term>Taux dissolution</term>
<term>Etude expérimentale</term>
<term>Oxygène</term>
<term>Astate</term>
<term>PH</term>
<term>Indium</term>
<term>Iode</term>
<term>Carbone</term>
<term>Transport</term>
<term>Dissolution</term>
<term>Béryllium</term>
<term>Mercure</term>
<term>Adsorption</term>
<term>Hydrodynamique</term>
<term>Altération météorique</term>
<term>Eau surface</term>
<term>Hydrochimie</term>
</keywords>
<keywords scheme="Wicri" type="concept" xml:lang="fr"><term>Oxygène</term>
<term>Iode</term>
<term>Carbone</term>
<term>Béryllium</term>
<term>Mercure</term>
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<front><div type="abstract" xml:lang="fr">The oxidative dissolution rate of metacinnabar by dissolved O<sub>2</sub>
was measured at pH ∼5 in batch and column reactors. In the batch reactors, the dissolution rate varied from 3.15 (±0.40) to 5.87 (±0.39) × 10<sup>-2</sup>
μmol/m<sup>2</sup>
/day (I = 0.01 M, 23°C) and increased with stirring speed, a characteristic normally associated with a transport-controlled reaction. However, theoretical calculations, a measured activation energy of 77 (±8) kJ/mol (I = 0.01 M), and the mineral dis-solution literature indicate reaction rates this slow are unlikely to be transport controlled. This phenomenon was attributed to the tendency of the hydrophobic source powder to aggregate and minimize the effective outer surface area. However, in a column experiment, the steady-state dissolution rate ranged from 1.34 (±0.11) to 2.27 (±0.11)x 10<sup>-2</sup>
μmol/m<sup>2</sup>
/day (I = 0.01 M, 23°C) and was also influenced by flow rate, suggesting hydrodynamic conditions may influence weathering rates observed in the field. The rate of Hg release to solution, under a range of hydrogeochemical conditions that more closely approximated those in the subsurface, was 1 to 3 orders of magnitude lower than the conditions that more closely approximated those in the subsurface, was 1 to 3 orders of magnitude lower than the dissolution rate due to the adsorption of released Hg(II) to the metacinnabar surface. The measured dissolution rates under all conditions were slow compared to the dissolution rates of minerals typically considered stable in the environment, and the adsorption of Hg(II) to the metacinnabar surface further lowered the Hg release rate.</div>
</front>
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<fA08 i1="01" i2="1" l="ENG"><s1>Oxidative dissolution of metacinnabar (β-HgS) by dissolved oxygen</s1>
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<fA11 i1="01" i2="1"><s1>BARNETT (Mark O.)</s1>
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<fA11 i1="02" i2="1"><s1>TURNER (Ralph R.)</s1>
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<fA11 i1="03" i2="1"><s1>SINGER (Philip C.)</s1>
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<fA14 i1="01"><s1>Environmental Sciences Division, Oak Ridge National Laboratory Oak Ridge</s1>
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<s3>USA</s3>
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<sZ>2 aut.</sZ>
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<sZ>3 aut.</sZ>
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<fC01 i1="01" l="FRE"><s0>The oxidative dissolution rate of metacinnabar by dissolved O<sub>2</sub>
was measured at pH ∼5 in batch and column reactors. In the batch reactors, the dissolution rate varied from 3.15 (±0.40) to 5.87 (±0.39) × 10<sup>-2</sup>
μmol/m<sup>2</sup>
/day (I = 0.01 M, 23°C) and increased with stirring speed, a characteristic normally associated with a transport-controlled reaction. However, theoretical calculations, a measured activation energy of 77 (±8) kJ/mol (I = 0.01 M), and the mineral dis-solution literature indicate reaction rates this slow are unlikely to be transport controlled. This phenomenon was attributed to the tendency of the hydrophobic source powder to aggregate and minimize the effective outer surface area. However, in a column experiment, the steady-state dissolution rate ranged from 1.34 (±0.11) to 2.27 (±0.11)x 10<sup>-2</sup>
μmol/m<sup>2</sup>
/day (I = 0.01 M, 23°C) and was also influenced by flow rate, suggesting hydrodynamic conditions may influence weathering rates observed in the field. The rate of Hg release to solution, under a range of hydrogeochemical conditions that more closely approximated those in the subsurface, was 1 to 3 orders of magnitude lower than the conditions that more closely approximated those in the subsurface, was 1 to 3 orders of magnitude lower than the dissolution rate due to the adsorption of released Hg(II) to the metacinnabar surface. The measured dissolution rates under all conditions were slow compared to the dissolution rates of minerals typically considered stable in the environment, and the adsorption of Hg(II) to the metacinnabar surface further lowered the Hg release rate.</s0>
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<fC03 i1="01" i2="2" l="FRE"><s0>Sulfure</s0>
<s5>01</s5>
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<fC03 i1="01" i2="2" l="ENG"><s0>sulfides</s0>
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<s5>01</s5>
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<fC03 i1="02" i2="2" l="FRE"><s0>Metacinabre</s0>
<s2>NZ</s2>
<s5>03</s5>
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<fC03 i1="02" i2="2" l="ENG"><s0>metacinnabar</s0>
<s2>NZ</s2>
<s5>03</s5>
</fC03>
<fC03 i1="02" i2="2" l="SPA"><s0>Metacinabrio</s0>
<s2>NZ</s2>
<s5>03</s5>
</fC03>
<fC03 i1="03" i2="2" l="FRE"><s0>Taux dissolution</s0>
<s5>06</s5>
</fC03>
<fC03 i1="03" i2="2" l="ENG"><s0>solution rates</s0>
<s5>06</s5>
</fC03>
<fC03 i1="03" i2="2" l="SPA"><s0>Proporción material disuelto</s0>
<s5>06</s5>
</fC03>
<fC03 i1="04" i2="2" l="FRE"><s0>Etude expérimentale</s0>
<s5>07</s5>
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<fC03 i1="04" i2="2" l="ENG"><s0>experimental studies</s0>
<s5>07</s5>
</fC03>
<fC03 i1="05" i2="2" l="FRE"><s0>Oxygène</s0>
<s5>08</s5>
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<fC03 i1="05" i2="2" l="ENG"><s0>oxygen</s0>
<s5>08</s5>
</fC03>
<fC03 i1="05" i2="2" l="SPA"><s0>Oxígeno</s0>
<s5>08</s5>
</fC03>
<fC03 i1="06" i2="2" l="FRE"><s0>Astate</s0>
<s5>09</s5>
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<fC03 i1="06" i2="2" l="ENG"><s0>astatine</s0>
<s5>09</s5>
</fC03>
<fC03 i1="06" i2="2" l="SPA"><s0>Astato</s0>
<s5>09</s5>
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<fC03 i1="07" i2="2" l="FRE"><s0>PH</s0>
<s5>10</s5>
</fC03>
<fC03 i1="07" i2="2" l="ENG"><s0>pH</s0>
<s5>10</s5>
</fC03>
<fC03 i1="07" i2="2" l="SPA"><s0>pH</s0>
<s5>10</s5>
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<fC03 i1="08" i2="2" l="FRE"><s0>Indium</s0>
<s5>11</s5>
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<fC03 i1="08" i2="2" l="ENG"><s0>indium</s0>
<s5>11</s5>
</fC03>
<fC03 i1="08" i2="2" l="SPA"><s0>Indio</s0>
<s5>11</s5>
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<s5>12</s5>
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<s5>12</s5>
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<s5>12</s5>
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<s5>13</s5>
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<s5>13</s5>
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<fC03 i1="10" i2="2" l="SPA"><s0>Carbono</s0>
<s5>13</s5>
</fC03>
<fC03 i1="11" i2="2" l="FRE"><s0>Transport</s0>
<s5>15</s5>
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<fC03 i1="11" i2="2" l="ENG"><s0>transport</s0>
<s5>15</s5>
</fC03>
<fC03 i1="11" i2="2" l="SPA"><s0>Transporte</s0>
<s5>15</s5>
</fC03>
<fC03 i1="12" i2="2" l="FRE"><s0>Dissolution</s0>
<s5>17</s5>
</fC03>
<fC03 i1="12" i2="2" l="ENG"><s0>dissolution</s0>
<s5>17</s5>
</fC03>
<fC03 i1="12" i2="2" l="SPA"><s0>Disolución</s0>
<s5>17</s5>
</fC03>
<fC03 i1="13" i2="2" l="FRE"><s0>Béryllium</s0>
<s5>18</s5>
</fC03>
<fC03 i1="13" i2="2" l="ENG"><s0>beryllium</s0>
<s5>18</s5>
</fC03>
<fC03 i1="13" i2="2" l="SPA"><s0>Berilio</s0>
<s5>18</s5>
</fC03>
<fC03 i1="14" i2="2" l="FRE"><s0>Mercure</s0>
<s5>21</s5>
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<fC03 i1="14" i2="2" l="ENG"><s0>mercury</s0>
<s5>21</s5>
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<fC03 i1="14" i2="2" l="SPA"><s0>Mercurio</s0>
<s5>21</s5>
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<s5>23</s5>
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<s5>61</s5>
</fC03>
<fC03 i1="17" i2="2" l="FRE"><s0>Altération météorique</s0>
<s5>62</s5>
</fC03>
<fC03 i1="17" i2="2" l="ENG"><s0>weathering</s0>
<s5>62</s5>
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<fC03 i1="17" i2="2" l="SPA"><s0>Alteración meteórica</s0>
<s5>62</s5>
</fC03>
<fC03 i1="18" i2="2" l="FRE"><s0>Eau surface</s0>
<s5>63</s5>
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<fC03 i1="18" i2="2" l="ENG"><s0>surface water</s0>
<s5>63</s5>
</fC03>
<fC03 i1="18" i2="2" l="SPA"><s0>Agua superficie</s0>
<s5>63</s5>
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<fC03 i1="19" i2="2" l="FRE"><s0>Hydrochimie</s0>
<s5>64</s5>
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<fC03 i1="19" i2="2" l="ENG"><s0>hydrochemistry</s0>
<s5>64</s5>
</fC03>
<fC03 i1="19" i2="2" l="SPA"><s0>Hidroquímica</s0>
<s5>64</s5>
</fC03>
<fC06><s0>ILS</s0>
<s0>TAS</s0>
<s0>ANS</s0>
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<fN21><s1>344</s1>
</fN21>
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