COF 衍生的多孔氮掺杂碳用于去除新兴有机污染物和从海水中高效提取铀。

COF-derived porous nitrogen-doped carbon for removal of emerging organic contaminants and efficient uranium extraction from seawater.

机构信息

MOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing, 102206, PR China.

Hebei Key Lab of Power Plant Flue Gas Multi-Pollutants Control, Department of Environmental Science and Engineering, North China Electric Power University, Baoding, 071003, PR China.

出版信息

Chemosphere. 2024 Oct;365:143354. doi: 10.1016/j.chemosphere.2024.143354. Epub 2024 Sep 16.

Abstract

The development of adsorbents for efficient and highly selective seawater extraction of uranium was instrumental in fostering sustainable progress in energy and addressing the prevailing energy crisis. However, the complex background composition of the marine environment, including radionuclides, organic pollutants, and a large number of co-existing heavy metal ions, were non-negligible obstacles to the extraction of uranium from seawater. The present investigation successfully employed a self-templated approach to synthesize porous nitrogen-doped carbon (PNC) derived from COF, which exhibited tremendous potential as an adsorbent for pollutant removal in environmental treatment. LZU1@PNC not only retained the structural features of the original COF-LZU1, but also overcame the acid-base instability problem commonly found in COFs. Subsequently, the removal process of two typical water pollutants on the material was investigated using 2,4-DCP and [UO(CO)]. The results demonstrated that LZU1@PNC exhibited superior removal performance for the target pollutants compared to COF-LZU1, owing to its larger specific surface area and abundant defect structure. After six desorption-regeneration cycles, LZU1@PNC still maintained a high removal rate of the target contaminants, demonstrating the stability of this material and its excellent recyclability. In addition, based on various characterization techniques, the removal mechanism of 2,4-DCP was presumed to be mainly electrostatic attraction, hydrogen bonding, and π-π stacking interactions. Conversely, the elimination process of [UO(CO)] predominantly relied on surface complexation phenomena. The present investigation provided new perspectives and stimulated a broader study of other COF-derived carbon materials and their modifications as adsorbents for uranium extraction from seawater and other applications.

摘要

高效、高选择性吸附剂的开发对于促进能源的可持续发展和解决当前的能源危机具有重要意义。然而,海洋环境的复杂背景组成,包括放射性核素、有机污染物和大量共存的重金属离子,是从海水中提取铀的不可忽视的障碍。本研究成功地采用了自模板法合成了源于 COF 的多孔氮掺杂碳(PNC),作为环境处理中污染物去除的吸附剂具有巨大的潜力。LZU1@PNC 不仅保留了原始 COF-LZU1 的结构特征,而且克服了 COF 中常见的酸碱不稳定性问题。随后,使用 2,4-DCP 和[UO(CO)]研究了材料对两种典型水污染物的去除过程。结果表明,与 COF-LZU1 相比,LZU1@PNC 对目标污染物具有更好的去除性能,这归因于其更大的比表面积和丰富的缺陷结构。经过六次解吸-再生循环后,LZU1@PNC 仍能保持对目标污染物的高去除率,证明了该材料的稳定性和良好的可回收性。此外,基于各种表征技术,推测 2,4-DCP 的去除机制主要是静电吸引、氢键和π-π堆积相互作用。相反,[UO(CO)]的消除过程主要依赖于表面络合现象。本研究为其他 COF 衍生碳材料及其作为从海水中提取铀和其他应用的吸附剂的修饰提供了新的视角,并激发了更广泛的研究。

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