Zandi Pegah, Phani Arindam, Kim Seonghwan
Department of Mechanical and Manufacturing Engineering, University of Calgary, Calgary, Alberta, T2N 1N4, Canada.
Adv Mater. 2025 Jul;37(29):e2504142. doi: 10.1002/adma.202504142. Epub 2025 May 2.
Hexavalent chromium (Cr) ions in drinking water pose a significant risk to human health, being a leading cause for neurological disorders, organ damage, and infertility. This study introduces an ultrasensitive method for detecting trace Cr over a wide concentration range (≈ 100 pM - 100 µM) through fluorescence enhancement signatures via integration of both covalent and non-covalent interaction strategies on carbon quantum dots (CQD). The covalent functionalization is achieved from dual-functionalized CQD (CQD-(NH, COOH)) derived from coffee-waste. Additionally, the covalent and non-covalent approach integrates CQD-(NH, COOH) with graphitic carbon nitride (g-CN) to form a 2D/2D heterostructure. The synergy between CQD-(NH, COOH) and g-CN introduces a mid-gap band in their band structure, allowing multiple carrier excitation and recombination states, significantly enhancing the fluorescence quenching signal. This combination allows to achieve Cr detection sensitivity down to ≈100 pM concentration-matching the World Health Organization's 96 pM permissible limit of total Cr in drinking water. Furthermore, a 70 pM detection limit is reported for Cr in a mixture of twelve ions, including cations and anions, surpassing current state-of-the-art detection limits. These results highlight the potential of dual covalent and non-covalent modification strategy in nanomaterials to set new standards in ultrasensitive and wide-range fluorescent sensing applications.
饮用水中的六价铬(Cr)离子对人类健康构成重大风险,是导致神经紊乱、器官损伤和不孕不育的主要原因。本研究介绍了一种超灵敏方法,通过在碳量子点(CQD)上整合共价和非共价相互作用策略,利用荧光增强特征在宽浓度范围(约100 pM - 100 μM)内检测痕量Cr。共价功能化是通过由咖啡渣衍生的双功能化CQD(CQD-(NH, COOH))实现的。此外,共价和非共价方法将CQD-(NH, COOH)与石墨相氮化碳(g-CN)整合形成二维/二维异质结构。CQD-(NH, COOH)与g-CN之间的协同作用在其能带结构中引入了一个中间能隙带,允许多种载流子激发和复合状态,显著增强荧光猝灭信号。这种组合能够实现低至约100 pM浓度的Cr检测——与世界卫生组织规定的饮用水中总Cr的96 pM允许限值相匹配。此外,对于包含阳离子和阴离子的十二种离子混合物中的Cr,报告的检测限为70 pM,超过了当前的最先进检测限。这些结果突出了纳米材料中共价和非共价双重修饰策略在超灵敏和宽范围荧光传感应用中设定新标准的潜力。