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In-situ oxidized tungsten disulfide nanosheets achieve ultrafast photocatalytic extraction of uranium through hydroxyl-mediated binding and reduction
Nano Research ( IF 9.9 ) Pub Date : 2022-07-05 , DOI: 10.1007/s12274-022-4559-0
Huanhuan Liu , Jia Lei , Changyao Gong , Ye Li , Huimei Chen , Jiali Chen , Fengchun Wen , Dengjiang Fu , Yan Liu , Wenkun Zhu , Rong He

Photoreduction of hexavalent uranium (U(VI)) by semiconductor provides a novel and effective avenue for uranium extraction. Unfortunately, the traditional metal oxide and sulfide semiconductors suffer from the lack of confinement sites to U(VI), which resulted in the long period (∼ 1 h) to achieve a high U(VI) extraction efficiency of > 90%. Herein, we successfully constructed WS2 nanosheets and created in-situ oxidized domains on the surfaces (O-WS2) to promote the uranium extraction and the corresponding removal kinetics. In this system, the O7.7-WS2 nanosheets exhibited a considerable U(VI) extraction efficiency of > 90% within 20 min in 8 mg·L−1 U(VI)-containing solution, which represented the highly efficient U(VI) removal performance. In 200 mg·L−1 U(VI)-containing solution, the O7.7-WS2 nanosheets exhibited an extraction capacity of 652.4 mg·g−1. The mechanism study revealed that the oxidized surface tended to trap hydrogen atom and in-situ form hydroxyl groups in defect sites. Evidenced by a series of experiment, such as kinetic isotope effect, 1H nuclear magnetic resonance (NMR) spectra, and X-ray absorption near-edge structure (XANES) spectra, the in-situ formed hydroxyl groups participated in the uranium reduction, which dramatically enhanced uranium extraction kinetics and efficiency.



中文翻译:

原位氧化二硫化钨纳米片通过羟基介导的结合和还原实现铀的超快光催化提取

通过半导体光还原六价铀 (U(VI)) 为铀提取提供了一种新颖而有效的途径。不幸的是,传统的金属氧化物和硫化物半导体缺乏对 U(VI) 的限制位点,这导致需要很长的时间(~1 小时)才能实现 > 90% 的高 U(VI) 提取效率。在此,我们成功地构建了 WS 2纳米片并在表面上产生原位氧化域(O-WS 2)以促进铀提取和相应的去除动力学。在该系统中,O 7.7 -WS 2纳米片在 8 mg·L -1的 20 分钟内表现出相当大的 U(VI) 提取效率 > 90%含 U(VI) 的溶液,代表了高效的 U(VI) 去除性能。在200 mg·L -1 U(VI)的溶液中,O 7.7 -WS 2纳米片的萃取能力为652.4 mg·g -1。机理研究表明,氧化表面倾向于捕获氢原子并在缺陷位点原位形成羟基。动力学同位素效应、 1 H核磁共振(NMR)光谱、X射线吸收近边结构(XANES)光谱等一系列实验证明,原位形成的羟基参与了铀的还原,这极大地提高了铀提取动力学和效率。

更新日期:2022-07-07
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