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从放射性废水中合成铀单原子以增强水离解和析氢

Synthesis of Uranium Single Atom from Radioactive Wastewater for Enhanced Water Dissociation and Hydrogen Evolution.

作者信息

Liu Min, Chen Huimei, Tang Xingrui, Liu Huanhuan, Tu Boyuan, Guo Weicong, Zheng Yamin, Liu Yan, Tang Yongjian, 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, Faculty of Science Southwest University of Science and Technology, Southwest University of Science and Technology, Sichuan Mianyang, 621010, China.

School of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China.

出版信息

Small. 2022 Mar;18(11):e2107444. doi: 10.1002/smll.202107444. Epub 2022 Feb 7.

Abstract

As a common nuclide in radioactive wastewater, uranium (U) is generally treated by landfill, which induces the massive abandonment of uranium resources. In this work, a pulse voltammetry method for the synthesis of U single atoms on MoS (U/MoS ) nanosheets from radioactive wastewater for the electrocatalytic alkaline hydrogen evolution reaction (HER) is reported. The mass loading of U single atoms is facilely controlled with high selectivity for coexisting ions in radioactive wastewater. In the electrolyte of 1 m of KOH, U/MoS nanosheets with 5.2% of U single atoms exhibit relatively low overpotentials of 72 mV at 10 mA cm . The mechanistic study reveals that the HER on U/MoS includes the water dissociation on U single atoms to form OH* and H transfer from OH* to adjacent S-edge atoms. This procedure exhibits decreased activation energy for transition state in water dissociation and optimized Gibbs free energy for H* adsorption.

摘要

作为放射性废水中的一种常见核素,铀(U)通常通过填埋处理,这导致大量铀资源被废弃。在这项工作中,报道了一种脉冲伏安法,用于从放射性废水中在MoS(U/MoS)纳米片上合成U单原子,用于电催化碱性析氢反应(HER)。U单原子的质量负载易于控制,对放射性废水中的共存离子具有高选择性。在1 m KOH的电解质中,含有5.2% U单原子的U/MoS纳米片在10 mA cm时表现出相对较低的72 mV过电位。机理研究表明,U/MoS上的HER包括U单原子上的水离解形成OH以及H从OH转移到相邻的S边缘原子。该过程在水离解中表现出降低的过渡态活化能以及优化的H*吸附吉布斯自由能。

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