用于高效电化学海水提铀的氮/硫共掺杂炭纳米片OA北大核心CSTPCD
N/S co-doped carbon nanosheets for the efficient electrochemical extraction of uranium from seawater
碳基催化剂是最具潜力的电化学海水提铀材料之一,但其实际应用性能常受高昂成本与低催化活性限制.本文利用廉价的聚苯乙烯磺酸树脂与三聚氰胺为原料,结合低温水热处理与高温炭化,开发了一类具有高催化活性的氮/硫共掺杂炭纳米片(CNSs),进一步与聚偕胺肟(PAO)共混后制备出一种吸附-催化一体化海水提铀复合电极.得益于CNSs自身高导电性与杂原子掺杂带来的高催化活性,基于CNSs的复合电极能在-2 V的电位下将海水中的铀酰离子催化为易于回收的Na2O(UO3·H2O)x沉淀物,并能在1×103 mg L-1的高浓度铀加标海水中实现3 923.7 mg g-1的提取容量与98.1%的铀去除率.原位拉曼光谱表明,电化学提铀40 min内,复合电极表面出现大量的铀化合物.值得指出的是,即使在铀浓度极低的天然海水中,该复合电极仍能回收72.7%的铀,具有优异的应用前景.
Carbon-based catalysts are promising materials for the electrochemical extraction of uranium from seawater.However,their practical application is often limited by high cost and low catalytic activity.Using low-cost polystyrene sulfonic acid resin and melamine as raw materials,a class of nitrogen and sulfur co-doped carbon nanosheets(CNSs)with high catalytic activity has been developed by a low-temperature hydrothermal treatment and high-temperature carbonization.Because of their high conductivity and high catalytic activity,CNS-based electrodes can catalyze uranyl ions in seawater into easily recoverable Na2O(UO3H2O)x precipitates at-2 V,and achieve an extraction capacity of up to 3 923.7 mg g-1 with a uranium removal of 98.1%in uranium-spiked seawater(1.0×103 mg L-1).In situ Raman spectroscopy showed that a large number of uranium compounds appeared on the surface of the composite electrode within 40 min of extraction.The electrode also recovered 72.7%of the uranium in natural seawater,demonstrating excellent prospects for this application.This work provides a new approach into the design of low-cost,metal-free electrocatalysts for the efficient uranium extraction from natural seawater.
易锬;黄俊龙;岑宗恒;纪轶炜;刘绍鸿
中山大学化学学院,广东 广州 510006广东省人民医院,广东 广州 510080中山大学化学学院,广东 广州 510006中山大学化学学院,广东 广州 510006中山大学化学学院,广东 广州 510006
化学工程
炭纳米片海水提铀杂原子掺杂电催化
Carbon nanosheetsUranium extraction from seawaterHeteroatom dopingElectrocatalysis
《新型炭材料(中英文)》 2024 (6)
1108-1116,9
感谢国家自然科学基金项目(52172061)、广东省自然科学基金杰出青年项目(2024B1515020023)、中央高校基本科研业务费(23yxqntd002和231gbj004)以及广东省高等学校功能分子工程基础研究卓越中心的资助. National Natural Science Foundation of China(52172061)Natural Science Foundation of Guangdong(2024B1515020023)Fundamental Research Funds for the Central Universities(23yxqntd002,231gbj004).
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