干旱区生态环境知识资源中心(Arid): Origin of the isotopic composition of natural perchlorate: Experimental results for the impact of reaction pathway and initial ClOx reactant

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DOI	10.1016/j.gca.2021.06.039
	Origin of the isotopic composition of natural perchlorate: Experimental results for the impact of reaction pathway and initial ClOx reactant
	Estrada, Nubia L.; Anderson, Todd A.; Bohlke, J. K.; Gu, Baohua; Hatzinger, Paul B.; Mroczkowski, Stanley J.; Rao, Balaji; Sturchio, Neil C.; Jackson, W. Andrew
通讯作者	Jackson, WA (corresponding author), Texas Tech Univ, Lubbock, TX 79409 USA.
来源期刊	GEOCHIMICA ET COSMOCHIMICA ACTA
ISSN	0016-7037
EISSN	1872-9533
出版年	2021
卷号	311 页码:292-315
英文摘要	Natural perchlorate (ClO4-) exists in many places on Earth, in lunar regolith, meteorites, and on the surface of Mars. Terrestrial natural ClO4- has widely variable Cl and O stable isotopic compositions (delta Cl-37, delta O-18, Delta O-17). The delta O-18 and Delta O-17 values of ClO4- from the most hyper-arid locations co-vary. ClO4- from less arid areas has relatively little O-17 excess and poor Delta O-17-delta O-18 correlation. ClO4- from the Atacama Desert has unusually low delta Cl-37 (<-10 parts per thousand) and exhibits a positive correlation between delta Cl-37 and delta O-18, while the delta Cl-37 of ClO4- from all other locations varies between -5 and +7 parts per thousand with no delta Cl-37-delta O-18 covariation. To evaluate the impact of different precursors (ClOx) and reaction pathways on the isotopic composition of ClO4-, we measured the isotopic composition of ClO(4)(-)produced in the laboratory by UV or O-3 mediated aqueous oxidation of Cl-, OCl-, ClO2-, and ClO2 degrees as well as O-3 mediated oxidation of dry NaCl. ClOx oxidation in aqueous or dry systems enriched in O-3 produced ClO4- with Delta O-17 values that generally increased with the number of O atoms required and included evidence that the site-specific O-17 anomaly in O(3 )was preferentially transferred to ClO4-. Based on the inferred number of O atoms sourced from O-3, and known Cl and O reaction pathways, it appears that ClO2 degrees and ClO3* were required intermediates in the production of ClO4- in the O-3 experiments. ClOx aqueous oxidation by UV irradiation produced ClO(4)(- )with a large range of delta O-18 values and little or no O-17 anomaly. ClO3- was produced to a much greater extent than ClO4- in all experiments except dry oxidation of NaCl by O-3. The isotopic composition of ClO3- was distinct from that of ClO4- produced from the same initial reactants. Combined results of O-3 and UV mediated reactions largely bracketed the range of natural ClO4- delta O-18 and Delta O-17 values as well as delta Cl-37 values of non-Atacama natural samples, but no conditions produced the low delta Cl-37 values of Atacama ClO4-. 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 ClO(4)(- )and ClO3-. (C) 2021 Elsevier Ltd. All rights reserved.
英文关键词	Perchlorate Chlorate Oxyanions Stable isotopic composition Ozone Photolysis chlorine isotopes oxygen isotopes
类型	Article
语种	英语
收录类别	SCI-E
WOS记录号	WOS:000693443000006
WOS关键词	ATMOSPHERIC NITRATE ; TROPOSPHERIC OZONE ; MASS-BALANCE ; OXYGEN ; FRACTIONATION ; CHLORINE ; GROUNDWATER ; WATER ; DEPOSITION ; OXIDATION
WOS类目	Geochemistry & Geophysics
WOS研究方向	Geochemistry & Geophysics
来源机构	United States Geological Survey
资源类型	期刊论文
条目标识符	http://119.78.100.177/qdio/handle/2XILL650/363380
作者单位	[Estrada, Nubia L.; Anderson, Todd A.; Rao, Balaji; Jackson, W. Andrew] Texas Tech Univ, Lubbock, TX 79409 USA; [Bohlke, J. K.; Mroczkowski, Stanley J.] US Geol Survey, Reston, VA 20192 USA; [Gu, Baohua] Oak Ridge Natl Lab, POB 2009, Oak Ridge, TN 37831 USA; [Hatzinger, Paul B.] APTIM, Lawrenceville, NJ 08648 USA; [Sturchio, Neil C.] Univ Delaware, Newark, DE 19716 USA
推荐引用方式 GB/T 7714	Estrada, Nubia L.,Anderson, Todd A.,Bohlke, J. K.,et al. Origin of the isotopic composition of natural perchlorate: Experimental results for the impact of reaction pathway and initial ClOx reactant[J]. United States Geological Survey,2021,311:292-315.
APA	Estrada, Nubia L..,Anderson, Todd A..,Bohlke, J. K..,Gu, Baohua.,Hatzinger, Paul B..,...&Jackson, W. Andrew.(2021).Origin of the isotopic composition of natural perchlorate: Experimental results for the impact of reaction pathway and initial ClOx reactant.GEOCHIMICA ET COSMOCHIMICA ACTA,311,292-315.
MLA	Estrada, Nubia L.,et al."Origin of the isotopic composition of natural perchlorate: Experimental results for the impact of reaction pathway and initial ClOx reactant".GEOCHIMICA ET COSMOCHIMICA ACTA 311(2021):292-315.