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Mechanisms of arsenic-containing pyrite oxidation by aqueous arsenate under anoxic conditions
Qiu, Guohong1; Gao, Tianyu1; Hong, Jun1; Tan, Wenfeng1; Liu, Fan1; Zheng, Lirong2
刊名Geochimica et cosmochimica acta
2017-11-15
卷号217页码:306-319
关键词Arsenic-containing pyrite Arsenate Adsorption Redox Goethite
ISSN号0016-7037
DOI10.1016/j.gca.2017.08.030
通讯作者Qiu, guohong(qiugh@mail.hzau.edu.cn)
英文摘要Adsorption and redox reactions occur between arsenic-containing pyrite and arsenate, which affect the migration and conversion of arsenic in soils and waters. however, the influence of arsenic incorporated in pyrite on the interaction processes is still enigmatic. in this work, arsenic-containing pyrites were hydrothermally synthesized with composition similar to naturally surface-oxidized pyrites in supergene environments. the effects of arsenic incorporation on the chemical composition and physicochemical properties were analyzed, and the interaction mechanism between arsenic-containing pyrites and aqueous arsenate was also studied within ph 3.0-11.0. arsenic-containing pyrites with the arsenic contents of 0 (apy0), 4.4 (apy5) and 9.9 wt.% (apy10) were produced in hydrothermal systems. as(iii) and as(-i) respectively substituted fe(ii) and s-2(-ii) in the pyrite, and their relative contents respectively reached 76.6% and 17.2% in apy5, and 91.0% and 8.0% in apy10. arsenic substitution resulted in a high content of fe(iii) in the form of fe(iii) as and a decrease in pyrite crystallinity. during the redox processes of arsenic-containing pyrites and arsenate, elemental s-0, so42- and goethite were formed as the main products with the adsorption of as(iii, v), and as(iii) was released due to the collapse of the crystal structure of pyrite and the oxidation of as(-i). different redox mechanisms were achieved with ph increasing from 3.0 to 11.0 in the reaction system. at ph 3.0-6.0, fe(iii) contributed much to the oxidation of arsenic-containing pyrites, and arsenate and released as (iii) were adsorbed on the surface of solid products. at ph 7.0-11.0, aqueous arsenate worked as the major oxidant, and its oxidation capacity increased with increasing ph. when the ph was increased from 3.0 to 7.0 and 11.0, the release ratio of incorporated arsenic from apy10 particles increased from 34.1% to 45.0% and 56.8%, respectively. the present study facilitates a better understanding about the interaction mechanisms between arsenic-containing pyrite and arsenate in supergene environments. (c) 2017 elsevier ltd. all rights reserved.
WOS关键词X-RAY PHOTOELECTRON ; SYNTHETIC PYRITE ; ELECTRICAL-PROPERTIES ; ABIOTIC OXIDATION ; NI IMPURITIES ; SOLID-PHASES ; FES2 ; SPECIATION ; MACKINAWITE ; REDUCTION
WOS研究方向Geochemistry & Geophysics
WOS类目Geochemistry & Geophysics
语种英语
出版者PERGAMON-ELSEVIER SCIENCE LTD
WOS记录号WOS:000411362000018
内容类型期刊论文
URI标识http://www.corc.org.cn/handle/1471x/2177077
专题高能物理研究所
通讯作者Qiu, Guohong
作者单位1.Huazhong Agr Univ, Coll Resources & Environm, Minist Agr, Key Lab Arable Land Conservat Middle & Lower Reac, Wuhan 430070, Hubei, Peoples R China
2.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100039, Peoples R China
推荐引用方式
GB/T 7714
Qiu, Guohong,Gao, Tianyu,Hong, Jun,et al. Mechanisms of arsenic-containing pyrite oxidation by aqueous arsenate under anoxic conditions[J]. Geochimica et cosmochimica acta,2017,217:306-319.
APA Qiu, Guohong,Gao, Tianyu,Hong, Jun,Tan, Wenfeng,Liu, Fan,&Zheng, Lirong.(2017).Mechanisms of arsenic-containing pyrite oxidation by aqueous arsenate under anoxic conditions.Geochimica et cosmochimica acta,217,306-319.
MLA Qiu, Guohong,et al."Mechanisms of arsenic-containing pyrite oxidation by aqueous arsenate under anoxic conditions".Geochimica et cosmochimica acta 217(2017):306-319.
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