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基于商业可得的废聚丙烯腈纤维的新型复合材料的合成与表征,用于从 U(VI)-CO 溶液中有效去除铀酰。

Synthesis and characterization of waste commercially available polyacrylonitrile fiber-based new composites for efficient removal of uranyl from U(VI)-CO solutions.

机构信息

College of Nuclear Technology and Automation Engineering, Chengdu University of Technology, Chengdu 610059, P. R. China.

National Key Laboratory for Nuclear Fuel and Materials, Nuclear Power Institute of China, Chengdu 610005, P. R. China.

出版信息

Sci Total Environ. 2022 May 20;822:153507. doi: 10.1016/j.scitotenv.2022.153507. Epub 2022 Jan 29.

DOI:10.1016/j.scitotenv.2022.153507
PMID:35101504
Abstract

The existing species of uranium determines the design of novel sorbents towards uranium extraction from the natural waters. Herein, three composites based on waste commercially available polyacrylonitrile fiber (WPANF), namely WPANF/TiO·xHO, WPANF/CTAB-bentonite, and WPANF/NZVI, were first prepared and employed for the removal of U(VI) from the carbonate coexisted aqueous solutions. Among them, the WPANF/TiO·xHO exhibited the optimum sorption capacity of 40.6 mg·g (pH 8.0, C = 50 mg·L, and [CO] = 2 mmol·L), which is significantly greater than the WPANF/CTAB-bentonite (12.6 mg·g) and WPANF/NZVI (~10.3 mg·g). All sorption capacities decreased with the increases of initial pH, [NaCl], and [CO], due to the species transformation from UO(CO) and (UO)CO(OH) to UO(CO) that enhanced the electrostatic repulsion and the competitive sorption. The XPS analysis and DFT calculations indicated that in the composites, WPANF was a role in strengthening the mechanical properties of composites rather than the main sorption sites for uranyl carbonates. The sorption mechanisms were mainly involved in -OH group coordination, Br anions exchanges, and redox reactions. Desorption, reusability and U(VI) sorption test in the simulated seawater demonstrated that WPANF/TiO·xHO could be an alternative candidate for acquiring uranium resource. This work has screened the potential composites for U(VI) extraction from the natural waters, especially based on the practical U(VI) speciation, and provides a novel research approach for the removal of U(VI) towards U(VI)-CO systems.

摘要

现有的铀物种决定了新型吸附剂的设计,以从天然水中提取铀。在此,首次制备了三种基于商业上可用的废聚丙烯腈纤维(WPANF)的复合材料,即 WPANF/TiO·xHO、WPANF/CTAB-膨润土和 WPANF/NZVI,并将其用于从共存的碳酸盐水溶液中去除 U(VI)。其中,WPANF/TiO·xHO 表现出40.6 mg·g 的最佳吸附容量(pH 8.0、C = 50 mg·L 和[CO] = 2 mmol·L),明显大于 WPANF/CTAB-膨润土(12.6 mg·g)和 WPANF/NZVI(~10.3 mg·g)。所有吸附容量都随初始 pH、[NaCl]和[CO]的增加而降低,这是由于 UO(CO)和(UO)CO(OH)的物种转化为 UO(CO),增强了静电排斥和竞争吸附。XPS 分析和 DFT 计算表明,在复合材料中,WPANF 是增强复合材料力学性能的作用,而不是铀碳酸盐的主要吸附位点。吸附机制主要涉及-OH 基团配位、Br 阴离子交换和氧化还原反应。在模拟海水中的解吸、重复使用性和 U(VI)吸附测试表明,WPANF/TiO·xHO 可以作为从天然水中获取铀资源的替代候选物。这项工作筛选了从天然水中提取 U(VI)的潜在复合材料,特别是基于实际的 U(VI)形态,为去除 U(VI)-CO 体系中的 U(VI)提供了一种新的研究方法。

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