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铀酰阳离子与层状双氢氧化物纳米颗粒之间的相互作用:对核废水管理的启示

Interaction between Uranyl Cations and Layered Double Hydroxide Nanoparticles: Implications for Nuclear Wastewater Management.

作者信息

Péter Tamás, Takács Dóra, Sáringer Szilárd, Szerlauth Adél, Sajdik Kadosa, Galbács Gábor, Tomšič Matija, Shaw Samuel, Morris Katherine, Douglas Grant, Szilágyi István

机构信息

MTA-SZTE Lendület Biocolloids Research Group, Interdisciplinary Excellence Centre, University of Szeged, H-6720 Szeged, Hungary.

Department of Physical Chemistry and Materials Science, University of Szeged, H-6720 Szeged, Hungary.

出版信息

ACS ES T Water. 2024 Jun 11;4(7):3059-3067. doi: 10.1021/acsestwater.4c00313. eCollection 2024 Jul 12.

Abstract

Effective uranium (U) capture is required for the remediation of contaminated solutes associated with the nuclear fuel cycle, including fuel reprocessing effluents, decommissioning, or nuclear accident cleanup. Here, interactions between uranyl cations (UO ) and a Mg-Al layered double hydroxide (LDH) were investigated using two types of uranyl-bearing LDH colloids. The first (ULDH) was synthesized by coprecipitation with 10% of Mg substituted by UO . Alternatively, UO was added to a neoformed LDH to obtain the second uranyl-bearing LDH colloid (LDHU). In both the LDHU and ULDH colloid systems, schoepite (UO)O(OH)·12HO, was formed. The presence of U significantly reduced the size of both LDHU and ULDH compared to a reference LDH colloid. Surface charge and aggregation of the ULDH and LDHU colloids were compared in NaCl, NaCO, NaSiO, and NaPO solutions that are often present in nuclear wastewaters. Aggregation of ULDH and LDHU in the presence of NaSiO or NaPO promotes colloid restabilization. While the uranyl cation was not incorporated into the LDH structure, it influences nanoparticle growth in addition to imparting modified surface properties that affect aggregation. This has implications for radioactive waste disposals, where LDH, which can also incorporate a variety of other radionuclides, is used for remediation.

摘要

有效捕获铀(U)对于修复与核燃料循环相关的受污染溶质至关重要,这些溶质包括燃料后处理废水、退役或核事故清理产生的废水。在此,使用两种含铀的层状双氢氧化物(LDH)胶体研究了铀酰阳离子(UO )与镁铝层状双氢氧化物(LDH)之间的相互作用。第一种(ULDH)是通过共沉淀合成的,其中10%的镁被UO 取代。或者,将UO 添加到新形成的LDH中以获得第二种含铀酰的LDH胶体(LDHU)。在LDHU和ULDH胶体体系中,均形成了柱磷铀矿(UO)O(OH)·12HO。与参考LDH胶体相比,铀的存在显著减小了LDHU和ULDH的尺寸。在核废水中常存在的NaCl、NaCO、NaSiO和NaPO溶液中,比较了ULDH和LDHU胶体的表面电荷和聚集情况。在NaSiO或NaPO存在下,ULDH和LDHU的聚集促进了胶体的再稳定。虽然铀酰阳离子未掺入LDH结构中,但它除了赋予影响聚集的改性表面性质外,还影响纳米颗粒的生长。这对放射性废物处置具有重要意义,在放射性废物处置中,也可掺入多种其他放射性核素的LDH被用于修复。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/8e22/11656702/752a6f60e11e/ew4c00313_0001.jpg

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