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利用同位素分馏和地球化学数据对铀矿原地酸浸后自然衰减的研究。

Study of natural attenuation after acid in situ leaching of uranium mines using isotope fractionation and geochemical data.

作者信息

Liu Zhenzhong, Li Chunguang, Tan Kaixuan, Li Yongmei, Tan Wanyu, Li Xiqi, Zhang Chong, Meng Shuo, Liu Longcheng

机构信息

School of Resource Environment and Safety Engineering, University of South China, Hengyang 421001, PR China.

School of Resource Environment and Safety Engineering, University of South China, Hengyang 421001, PR China; China Institute of Atomic Energy, Beiing 102413, PR China; R&D Center of Radioactive Waste Treatment, Disposal and Modeling, University of South China, Hengyang 421001, PR China.

出版信息

Sci Total Environ. 2023 Mar 20;865:161033. doi: 10.1016/j.scitotenv.2022.161033. Epub 2022 Dec 24.

Abstract

Acid in situ leaching (AISL) is a subsurface mining approach suitable for low-grade ores which does not generate tailings, and has been adopted widely in uranium mining. However, this technique causes an extremely high concentration of contaminants at post-mining sites and in the surroundings soon after the mining ceases. As a potential AISL remediation strategy, natural attenuation has not been studied in detail. To address this problem, groundwater collected from 26 wells located within, adjacent, upgradient, and downgradient of a post-mining site were chosen to analyze the fate of U(VI), SO, δS, and δU, to reveal the main mechanisms governing the migration and attenuation of the dominant contaminants and the spatio-temporal evolutions of contaminants in the confined aquifer of the post-mining site. The δU values vary from -0.07 ‰ to 0.09 ‰ in the post-mining site and from -1.43 ‰ to 0.03 ‰ around the post-mining site. The δS values were found to vary from 3.3 ‰ to 6.2 ‰ in the post-mining site and from 6.0 ‰ to 11.0 ‰ around the post-mining site. Detailed analysis suggests that there are large differences between the range of isotopic composition variation and the range of pollutants concentration distribution, and the estimated Rayleigh isotope fractionation factor is 0.9994-0.9997 for uranium and 1.0032-1.0061 for sulfur. The isotope ratio of uranium and sulfur can be used to deduce the migration history of the contaminants and the irreversibility of the natural attenuation process in the anoxic confined aquifer. Combining the isotopic fractionation data for U and S with the concentrations of uranium and sulfate improved the accuracy of understanding of reducing conditions along the flow path. The study also indicated that as long as the geological conditions are favorable for redox reactions, natural attenuation could be used as a cost-effective remediation scheme.

摘要

原地酸浸(AISL)是一种适用于低品位矿石的地下采矿方法,不会产生尾矿,已在铀矿开采中广泛采用。然而,该技术在采矿停止后不久,会使采矿后场地及其周边地区的污染物浓度极高。作为一种潜在的原地酸浸修复策略,自然衰减尚未得到详细研究。为解决这一问题,选取了从一个采矿后场地内部、相邻、上游和下游的26口井采集的地下水,分析U(VI)、SO、δS和δU的归宿,以揭示控制主要污染物迁移和衰减的主要机制,以及采矿后场地承压含水层中污染物的时空演变。采矿后场地的δU值在-0.07‰至0.09‰之间,采矿后场地周边的δU值在-1.43‰至0.03‰之间。发现采矿后场地的δS值在3.3‰至6.2‰之间,采矿后场地周边的δS值在6.0‰至11.0‰之间。详细分析表明,同位素组成变化范围与污染物浓度分布范围之间存在很大差异,铀的瑞利同位素分馏系数估计为0.9994 - 0.9997,硫的瑞利同位素分馏系数为1.0032 - 1.0061。铀和硫的同位素比值可用于推断污染物的迁移历史以及缺氧承压含水层中自然衰减过程的不可逆性。将U和S的同位素分馏数据与铀和硫酸盐的浓度相结合,提高了对沿水流路径还原条件理解的准确性。该研究还表明,只要地质条件有利于氧化还原反应,自然衰减就可作为一种经济有效的修复方案。

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