Item talk:Q300705
From geokb
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"name": "Origin of the isotopic composition of natural perchlorate: Experimental results for the impact of reaction pathway and initial ClOx reactant",
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"name": "Geochimica et Cosmochimica Acta",
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"abstract": "Natural\u00a0perchlorate\u00a0(ClO4\u2212) exists in many places on Earth, in lunar\u00a0regolith,\u00a0meteorites, and on the surface of Mars. Terrestrial natural ClO4\u2212\u00a0has widely variable Cl and O stable\u00a0isotopic compositions\u00a0(\u03b437Cl, \u03b418O, \u039417O). The \u03b418O and \u039417O values of ClO4\u2212\u00a0from the most hyper-arid locations co-vary. ClO4\u2212\u00a0from less arid areas has relatively little\u00a017O excess and poor \u039417O-\u03b418O correlation. ClO4\u2212\u00a0from the Atacama Desert has unusually low \u03b437Cl (<\u221210\u2030) and exhibits a positive correlation between \u03b437Cl and \u03b418O, while the \u03b437Cl of ClO4\u2212\u00a0from all other locations varies between \u22125 and +7\u2030 with no \u03b437Cl-\u03b418O covariation. To evaluate the impact of different precursors (ClOx) and reaction pathways on the isotopic composition of ClO4\u2212, we measured the isotopic composition of ClO4\u2212\u00a0produced in the laboratory by UV or O3\u00a0mediated aqueous oxidation of Cl\u2212, OCl\u2212, ClO2\u2212, and ClO2\u00b0 as well as O3\u00a0mediated oxidation of dry NaCl. ClOx\u00a0oxidation in aqueous or dry systems enriched in O3\u00a0produced ClO4\u2212\u00a0with \u039417O values that generally increased with the number of O atoms required and included evidence that the site-specific\u00a017O anomaly in O3\u00a0was preferentially transferred to ClO4\u2212. Based on the inferred number of O atoms sourced from O3, and known Cl and O reaction pathways, it appears that ClO2\u00b0 and ClO3* were required intermediates in the production of ClO4\u2212\u00a0in the O3\u00a0experiments. ClOx\u00a0aqueous oxidation by UV irradiation produced ClO4\u2212\u00a0with a large range of \u03b418O values and little or no\u00a017O anomaly. ClO3\u2212\u00a0was produced to a much greater extent than ClO4\u2212\u00a0in all experiments except dry oxidation of NaCl by O3. The isotopic composition of ClO3\u2212\u00a0was distinct from that of ClO4\u2212\u00a0produced from the same initial reactants. Combined results of O3\u00a0and UV mediated reactions largely bracketed the range of natural ClO4\u2212\u00a0\u03b418O and \u039417O values as well as \u03b437Cl values of non-Atacama natural samples, but no conditions produced the low \u03b437Cl values of Atacama ClO4\u2212. Our results indicate that variation in production mechanisms, possibly combined with isotopically variable precursors, could be responsible for much of the observed isotopic variation in natural ClO4\u2212\u00a0and ClO3\u2212.",
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