首页|氮掺杂中空碳负载的高熵合金在电化学去除铀方面的性能及机理探究

氮掺杂中空碳负载的高熵合金在电化学去除铀方面的性能及机理探究

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本文通过离子交换法制备了氮掺杂中空碳负载的高熵合金(HEA@HNPC),并用作电催化剂应用于水溶液中铀的去除.制备的HEA@HNPC具有灵活多变的元素组成、易于调控的表面电子结构和丰富的催化活性位点.分别探究了HEA@HNPC在纯水和模拟地下水中对铀的去除性能.结果表明,HEA@HNPC电催化剂对铀的去除表现出快速的动力学、较大的萃取容量、优异的选择性及增强的循环使用性能,放大实验发现HEA@HNPC对模拟地下水中铀的去除效率高达381.6mgg-1 d-1.采用SEM、XRD和XPS对电化学产物分析发现,还原的U(Ⅳ)会与产生的CaCO3沉淀形成混合物以固体的形式析出,实现铀的高效连续去除.电化学循环伏安曲线(CV)发现HEA@HNPC表面产生的具有强还原性的H*ad物种是实现U(Ⅵ)→ U(Ⅳ)电还原的关键.这一发现为应用电化学技术去除水溶液中铀的机理研究提供了有意义的参考.
Efficient electrocatalytic uranium removal and potential mechanism by hollow nitrogen-doped porous carbon-supported high-entropy alloy
A hollow nitrogen-doped porous carbon-supported high-entropy alloy(HEA@HNPC)was successfully prepared by ion exchange and used as an electrocatalyst for the removal of uranium from an aqueous solution.The as-synthesized HEA@HNCC possessed the feature of flexible element composition,adjustable surface electronic structure,and plentiful catalytic active sites.The removal performance for uranyl by HEA@HNCC electrocatalyst from aqueous solution and simulated groundwater was investigated,respectively.The results showed that the HEA@HNPC electrocatalyst exhibited fast kinetics,large extraction capacity,excellent selectivity and enhanced recycling stability for uranium removal,and removal efficiency of uranium by HEA@HNPC was up to 381.6 mg g-1d-1 in scale-up experiments.SEM,XRD,and XPS were used to analyze the electrochemical products,and it could be found that the reduced U(Ⅳ)would form a mixture solid with the CaCO3 precipitation to achieve efficient and continuous removal of uranium from aqueous solution.The electrochemical cyclic voltammetry(CV)curve revealed that the H*ad with strong reducing properties generated on the HEA@HNCC surface was the key species for U(Ⅵ)→U(Ⅳ)electroreduction.This discovery provides a significant reference for the mechanism research of the uranium removal from aqueous solution by electrochemical technology.

HEA@HNPCelectrochemical technologyuranium removalmechanism research

刘晓露、肖慕良、韩莹莹、刘效潇、陈中山、杨慧、王祥科

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华北电力大学环境科学与工程学院,北京 102206

HEA@HNPC 电化学技术 铀去除 机理研究

国家自然科学基金

22276054

2024

中国科学(化学)
中国科学院

中国科学(化学)

CSTPCD北大核心
影响因子:0.685
ISSN:1674-7224
年,卷(期):2024.54(2)
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