水化学作用下离子交换和表面络合对高岭石吸附稀土的影响

IF 2.9 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Elmira Ramazanova, Neha Sharma, Elaine D. Flynn, Olwen Stagg, Jeffrey G. Catalano and Daniel E. Giammar*, 
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引用次数: 0

摘要

稀土元素(ree)是可再生能源、交通运输和电子产品背后的现代技术的关键组成部分,但目前的供应有限。全球稀土产量的很大一部分依赖于离子吸附矿床。这些矿床的稀土富集带高岭石丰度高,说明高岭石控制着稀土的地下运移。本研究旨在提高目前对不同水化学条件下REE与高岭石结合的认识。我们在不同的pH、电解质浓度、溶解无机碳(DIC)、低分子量有机酸(柠檬酸和草酸)和总稀土浓度条件下,对高岭石(KGa-2)和三种稀土(Nd、Dy和Yb)进行了批量实验。增加电解质浓度可抑制pH <下稀土元素的吸附;这表明在这些pH值下离子交换有助于吸附。在pH 7-8以上,DIC通过与重稀土形成强水络合物来影响吸附。柠檬酸在pH >下通过水络合作用降低稀土的吸附;5,但不影响pH <下的吸附;5. 表面络合模型通过两种机制捕捉了主要的吸附趋势:pH <下基面上离子交换;~ 6和内球表面在pH >边缘位置的络合;∼6。表面络合的平衡常数按Yb >的顺序增加;Dy祝辞Nd,表明对重稀土具有较高的吸附强度。该研究证明了水化学条件如何控制吸附机制,这可能决定稀土在富含高岭石的地下环境中的迁移率。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Adsorption of REEs to Kaolinite via Ion Exchange and Surface Complexation as a Function of Water Chemistry

Adsorption of REEs to Kaolinite via Ion Exchange and Surface Complexation as a Function of Water Chemistry

Rare earth elements (REEs) are critical components of modern technology behind renewable energy, transportation, and electronics but have a limited current supply. A substantial portion of global REE production relies on ion adsorption deposits. A high abundance of kaolinite in REE enrichment zones within these deposits suggests that kaolinite controls the subsurface migration of REEs. This study aimed to improve the current understanding of REE binding to kaolinite under varying water chemistry conditions. We conducted batch experiments with kaolinite (KGa-2) and three REEs (Nd, Dy, and Yb) at varying pH, electrolyte concentration, dissolved inorganic carbon (DIC), low molecular weight organic acids (citric and oxalic acids), and total REE concentration conditions. Increasing electrolyte concentration inhibits REE adsorption at pH < 7, suggesting that ion exchange contributes to adsorption at these pH values. DIC affects adsorption above pH 7–8 by forming strong aqueous complexes with heavy REEs. Citric acid decreases REE adsorption via aqueous complexation of REEs at pH > 5 but does not affect adsorption at pH < 5. The surface complexation model captures the main adsorption trends with two mechanisms: ion exchange on basal planes at pH < ∼6 and inner-sphere surface complexation to edge sites at pH > ∼6. Equilibrium constants for surface complexation increase in the order of Yb > Dy > Nd, indicating a higher strength of adsorption for heavy REEs. This study demonstrates how water chemistry conditions control the adsorption mechanisms that may determine the mobility of REEs in subsurface environments rich in kaolinite.

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来源期刊
ACS Earth and Space Chemistry
ACS Earth and Space Chemistry Earth and Planetary Sciences-Geochemistry and Petrology
CiteScore
5.30
自引率
11.80%
发文量
249
期刊介绍: The scope of ACS Earth and Space Chemistry includes the application of analytical, experimental and theoretical chemistry to investigate research questions relevant to the Earth and Space. The journal encompasses the highly interdisciplinary nature of research in this area, while emphasizing chemistry and chemical research tools as the unifying theme. The journal publishes broadly in the domains of high- and low-temperature geochemistry, atmospheric chemistry, marine chemistry, planetary chemistry, astrochemistry, and analytical geochemistry. ACS Earth and Space Chemistry publishes Articles, Letters, Reviews, and Features to provide flexible formats to readily communicate all aspects of research in these fields.
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