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在无金属的石墨相氮化碳上原位构建偕胺肟基团以增强化学吸附、光吸收和载流子分离,实现高效光辅助铀(VI)萃取。

In-situ constructing amidoxime groups on metal-free g-CN to enhance chemisorption, light absorption, and carrier separation for efficient photo-assisted uranium(VI) extraction.

作者信息

Yu Kaifu, Li Yi, Cao Xin, Wang Ruixiang, Zhou Li, Wu Linzhen, He Ningning, Lei Jia, Fu Dengjiang, Chen Tao, He Rong, Zhu Wenkun

机构信息

State Key Laboratory of Environment-friendly Energy Materials, National Co-innovation Center for Nuclear Waste Disposal and Environmental Safety, Sichuan Civil-military Integration Institute, School of National Defence & Nuclear Science and Technology, Southwest University of Science and Technology, Mianyang, Sichuan 621010, PR China; College of Chemistry, Sichuan University, Chengdu, Sichuan 610064, PR China.

School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, Heilongjiang 150001, PR China.

出版信息

J Hazard Mater. 2023 Oct 15;460:132356. doi: 10.1016/j.jhazmat.2023.132356. Epub 2023 Aug 22.

Abstract

The development of inexpensive and efficient semiconductor catalysts for photo-assisted uranium extraction from seawater remains a huge challenge. Herein, we have successfully synthesized amidoxime-rich g-CN (AO-CN) by simply amidoximing a cyano-rich precursor for photo-assisted uranium extraction from seawater. The amidoxime groups not only served as the U(VI) binding sites for efficient uranium adsorption, but also significantly improved the visible light absorption capacity and carrier separation efficiency via introducing defect energy level, resulting in the excellent photocatalytic activity for AO-CN towards photo-assisted uranium extraction. In the process of photo-assisted uranium extraction, U(VI) was first adsorbed by the amidoxime groups on the AO-CN and then reduced to U(IV), while (UO)O·2HO and (UO)O·4HO were further formed by the oxidation of U(IV) by superoxide radicals (·O). Moreover, the generated reactive oxygen species (ROS) under light endowed AO-CN with outstanding antibacterial properties, preventing the limitation of uranium extraction capacity from marine biofouling.

摘要

开发用于光辅助从海水中提取铀的廉价高效半导体催化剂仍然是一个巨大的挑战。在此,我们通过简单地将富含氰基的前驱体氨肟化,成功合成了富含偕胺肟的石墨相氮化碳(AO-CN),用于光辅助从海水中提取铀。偕胺肟基团不仅作为U(VI)的结合位点实现高效铀吸附,还通过引入缺陷能级显著提高了可见光吸收能力和载流子分离效率,从而使AO-CN对光辅助铀提取具有优异的光催化活性。在光辅助铀提取过程中,U(VI)首先被AO-CN上的偕胺肟基团吸附,然后还原为U(IV),而超氧自由基(·O)将U(IV)氧化进一步形成(UO)O·2HO和(UO)O·4HO。此外,光照下产生的活性氧(ROS)赋予AO-CN出色的抗菌性能,避免了海洋生物污染对铀提取能力的限制。

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