Reduction of uranium (VI) in water with additive manufactured electrode

IF 4.1 3区 化学 Q1 CHEMISTRY, ANALYTICAL Journal of Electroanalytical Chemistry Pub Date : 2025-03-15 Epub Date: 2025-02-09 DOI:10.1016/j.jelechem.2025.119005
Florent Belnou , Michel L. Schlegel , Thomas Proslier , Julie Mayounove , Hicham Maskrot
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Abstract

Nuclear energy has a promising future, but conventional uranium resources are expected to be depleted within a century. Electrochemical extraction could overcome this roadblock by quantitatively recovering uranium dissolved in natural waters using high surface-area electrodes. In this paper, 3D-architected electrodes were manufactured and studied in an electrochemical cell for element extraction. First, untreated flat electrodes made by Laser Powder Bed Fusion (LPBF) and studied by Cyclic Voltammetry (CV) with a custom electrochemical flow cell in a solution of 1 mM Fe(III)(CN)63−, 0.1 M KCl have exhibited a shift in redox waves because of an oxidized surface. After electro-etching of the electrode surface with oxalic acid, CV exhibited wave positions closer to literature values with higher amplitudes. However, with a solution of 10−3 M uranium, 0.1 M NaCl with a pH of 2.3, no electrochemical signals were detected. In contrast, uranium electrochemically reacted with, and was quantitatively retained by an electrode coated with 10 nm of TiO2 by Atomic Layer Deposition (ALD), and the electrode surface was able to retain uranium by chronoamperometry (CA) (about 0.5 mg for a surface of 3.0 cm2). To increase the reacting surface, 3D-architected electrodes were manufactured, electro-etched and TiO2-coated. These electrodes showed a tenfold increase in uranium retention (up to 5.7 mg for a surface of 111.1 cm2) that could be partially re-dissolved in a new solution with a yield of 70 %. This work shows the interest of both surface functionalization and architected electrodes for elemental retention.

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用添加剂制造电极还原水中铀(VI)
核能前景光明,但传统的铀资源预计将在一个世纪内耗尽。电化学萃取可以通过使用高表面积电极定量回收溶解在自然水中的铀来克服这一障碍。本文制作了三维结构电极,并在电化学电池中进行了元素提取的研究。首先,在1 mM Fe(III)(CN)63−,0.1 M KCl溶液中,采用激光粉末床熔合(LPBF)制作的未经处理的扁平电极,通过循环伏安法(CV)在定制的电化学流动电池中进行了研究,发现由于表面氧化,氧化还原波发生了移位。用草酸对电极表面进行电蚀刻后,CV的波位更接近文献值,振幅更高。而在10−3 M铀、0.1 M NaCl、pH = 2.3的溶液中,没有检测到电化学信号。相比之下,铀与原子层沉积法(ALD)包覆10 nm TiO2的电极发生电化学反应并被定量保留,通过计时电流法(CA),电极表面能够保留铀(3.0 cm2表面约0.5 mg)。为了增加反应表面,制造了3d结构电极,电蚀刻和二氧化钛涂层。这些电极显示铀的保留量增加了10倍(在111.1 cm2的表面上高达5.7 mg),可以部分地在新溶液中再溶解,收率为70%。这项工作显示了表面功能化和结构电极对元素保留的兴趣。
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来源期刊
CiteScore
7.80
自引率
6.70%
发文量
912
审稿时长
2.4 months
期刊介绍: The Journal of Electroanalytical Chemistry is the foremost international journal devoted to the interdisciplinary subject of electrochemistry in all its aspects, theoretical as well as applied. Electrochemistry is a wide ranging area that is in a state of continuous evolution. Rather than compiling a long list of topics covered by the Journal, the editors would like to draw particular attention to the key issues of novelty, topicality and quality. Papers should present new and interesting electrochemical science in a way that is accessible to the reader. The presentation and discussion should be at a level that is consistent with the international status of the Journal. Reports describing the application of well-established techniques to problems that are essentially technical will not be accepted. Similarly, papers that report observations but fail to provide adequate interpretation will be rejected by the Editors. Papers dealing with technical electrochemistry should be submitted to other specialist journals unless the authors can show that their work provides substantially new insights into electrochemical processes.
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