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通过调控普鲁士蓝类似物衍生吸附剂中的丰富活性氧位实现高效 Yb(III)捕获。

Tailoring abundant active-oxygen sites of Prussian blue analogues-derived adsorbents for highly efficient Yb(III) capture.

机构信息

Key Laboratory of Green Chemical Process of Ministry of Education, Hubei Key Laboratory for Novel Reactor and Green Chemical Technology, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430073, China; Key Laboratory of Coal Processing and Efficient Utilization, (China University of Mining and Technology), Ministry of Education, Xuzhou 221008, China.

Key Laboratory of Green Chemical Process of Ministry of Education, Hubei Key Laboratory for Novel Reactor and Green Chemical Technology, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430073, China.

出版信息

J Hazard Mater. 2023 Mar 5;445:130457. doi: 10.1016/j.jhazmat.2022.130457. Epub 2022 Nov 21.

DOI:10.1016/j.jhazmat.2022.130457
PMID:36444809
Abstract

The removal of rare earth elements in mineral processing wastewater is highly desirable but still challenging. In this study, three bimetallic Prussian blue analogues (PBA) and six corresponding oxides are prepared by co-precipitation and calcination methods, and then utilized to adsorb aqueous Yb(III) solution. The results of XRD, SEM, BET, and XPS indicate the successful synthesis of all the adsorbents. Among them, three PBA-oxide samples (PBO-800) exhibit the superior adsorption capacities (˃250 mg/g). The adsorption processes of Yb(III) are in accordance with the pseudo-second-order kinetic model and Langmuir model, simultaneously showing the spontaneous and endothermic thermodynamics. Moreover, PBO-800 can be reused after alkaline solution regeneration with less than 10% degradation after five consecutive adsorption-desorption cycles. More importantly, PBO-800 exhibits the impressive separation selectivity of Yb(III) and most light rare earth ions (e.g., 5.51 of Yb/La, 4.03 of Yb/Pr), as well as the selectivity of Yb(III) and alkali metal ions (e.g., 300.5 of Yb/Na, 256.2 of Yb/Ca). According to the characterization analysis and DFT calculation, the adsorption mechanism of Yb(III) by PBO-800 is mainly attributed to the strong interaction between the abundant active-oxygen sites and Yb(III), and the significant electrostatic attraction.

摘要

从矿物加工废水中去除稀土元素是非常理想的,但仍然具有挑战性。在这项研究中,通过共沉淀和煅烧方法制备了三种双金属普鲁士蓝类似物(PBA)和六种相应的氧化物,并将其用于吸附水溶液中的 Yb(III)溶液。XRD、SEM、BET 和 XPS 的结果表明所有吸附剂都成功合成。其中,三种 PBA-氧化物样品(PBO-800)表现出优越的吸附能力(>250mg/g)。Yb(III)的吸附过程符合准二级动力学模型和 Langmuir 模型,同时表现出自发和吸热的热力学。此外,PBO-800 可以在碱性溶液再生后重复使用,经过五个连续的吸附-解吸循环后,降解率低于 10%。更重要的是,PBO-800 对 Yb(III)和大多数轻稀土离子(例如,Yb/La 的 5.51,Yb/Pr 的 4.03)表现出令人印象深刻的分离选择性,以及对 Yb(III)和碱金属离子(例如,Yb/Na 的 300.5,Yb/Ca 的 256.2)的选择性。根据表征分析和 DFT 计算,PBO-800 吸附 Yb(III)的机制主要归因于丰富的活性氧位与 Yb(III)之间的强相互作用,以及显著的静电吸引力。

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