Silver Nanoparticle-Grafted Amidoxime Covalent Organic Framework: A Highly Sensitive and Selective SERS Substrate for Uranium Detection in Natural Water Systems

IF 19 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Xintong Guo, Xueyu Wang, Shizheng Wen, Huazhen Wu, Jing Wang, Mei Wang, Dewen He, Fuqiang Zhao, Jiakai Liu, Xueqing Yang, Shuao Wang
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Abstract

Uranium is a critical nuclear material and a significant environmental contaminant due to its high toxicity, making its detection important. Surface-enhanced Raman Scattering (SERS) has been used for the rapid and sensitive analysis of uranyl, but achieving both high sensitivity and selectivity in natural water systems remains a challenge. Herein, a novel Ag@COF-TpDb-AO substrate by depositing silver nanoparticles (AgNPs) onto amidoxime groups functionalized ketoenamine-based covalent organic framework (COF-TpDb-AO) for uranyl detection is fabricated. This method achieves a low detection limit of 3.72 µg L⁻¹, significantly below the World Health Organization (WHO) maximum contamination standard of 30 µg L⁻¹ in drinking water. It also demonstrates a high enhancement factor of 1.26 × 10⁶, excellent interference resistance, reproducibility, and stability. Importantly, this method can detect uranyl in practical samples, including tap, river, and lake water, with recoveries ranging from 93.1% to 104.8%. The detection capability arises from the adsorption of trace uranyl onto COF-TpDb-AO, followed by enhancement of Raman intensity through electromagnetic and chemical synergistic effects. The enhancement mechanism is demonstrated by Finite-Difference Time-Domain (FDTD) and Density Functional Theory (DFT) calculations. This study presents a novel SERS substrate for trace uranyl detection in natural water systems, paving the way for improved environmental monitoring.

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银纳米颗粒接枝偕胺肟共价有机骨架:用于天然水体中铀检测的高灵敏度和选择性SERS底物
铀是一种重要的核材料,也是一种重要的环境污染物,由于其高毒性,因此对其进行检测非常重要。表面增强拉曼散射(SERS)已被用于铀酰的快速灵敏分析,但在天然水系统中实现高灵敏度和高选择性仍然是一个挑战。本文通过将银纳米颗粒(AgNPs)沉积在偕胺肟基功能化酮胺基共价有机框架(COF-TpDb-AO)上,制备了一种用于铀酰检测的新型Ag@COF-TpDb-AO底物。该方法的检测限低至3.72µg L -⁻,大大低于世界卫生组织(WHO)饮用水中30µg L -⁻的最大污染标准。它还具有1.26 × 10 6的高增强因子,具有良好的抗干扰性、重现性和稳定性。重要的是,该方法可以在自来水、河水和湖水等实际样品中检测铀酰,回收率为93.1% ~ 104.8%。COF-TpDb-AO吸附微量铀酰后,通过电磁和化学协同作用增强拉曼强度,从而提高了检测能力。通过时域有限差分(FDTD)和密度泛函理论(DFT)的计算证明了增强机理。本研究提出了一种用于天然水体中痕量铀酰检测的新型SERS底物,为改善环境监测铺平了道路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Advanced Functional Materials
Advanced Functional Materials 工程技术-材料科学:综合
CiteScore
29.50
自引率
4.20%
发文量
2086
审稿时长
2.1 months
期刊介绍: Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week. Advanced Functional Materials is known for its rapid and fair peer review, quality content, and high impact, making it the first choice of the international materials science community.
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