Norton Amie E, Sharma Malvika, Cashen Christina, Dourges Marie-Anne, Toupance Thierry, Krause Jeanette A, Motkuri Radha Kishan, Connick William B, Chatterjee Sayandev
Department of Chemistry, University of Cincinnati, P.O. Box 210172, Cincinnati, Ohio 45221, United States.
University of Bordeaux, Institute of Molecular Chemistry, UMR 5255 CNRS, 351 Cours de la Libération, F-33405 Talence Cédex, France.
ACS Appl Mater Interfaces. 2021 Apr 14;13(14):16197-16209. doi: 10.1021/acsami.0c20821. Epub 2021 Mar 31.
Increased levels of nitrate (NO) in the environment can be detrimental to human health. Herein, we report a robust, cost-effective, and scalable, hybrid material-based colorimetric/luminescent sensor technology for rapid, selective, sensitive, and interference-free NO detection. These hybrid materials are based on a square-planar platinum(II) salt [Pt(tpy)Cl]PF (tpy = 2,2';6',2″-terpyridine) supported on mesoporous silica. The platinum salt undergoes a vivid change in color and luminescence upon exposure to aqueous NO anions at pH ≤ 0 caused by substitution of the PF anions by aqueous NO. This change in photophysics of the platinum salt is induced by a rearrangement of its crystal lattice that leads to an extended Pt···Pt···Pt interaction, along with a concomitant change in its electronic structure. Furthermore, incorporating the material into mesoporous silica enhances the surface area and increases the detection sensitivity. A NO detection limit of 0.05 mM (3.1 ppm) is achieved, which is sufficiently lower than the ambient water quality limit of 0.16 mM (10 ppm) set by the United States Environmental Protection Agency. The colorimetric/luminescence of the hybrid material is highly selective to aqueous NO anions in the presence of other interfering anions, suggesting that this material is a promising candidate for the rapid NO detection and quantification in practical samples without separation, concentration, or other pretreatment steps.
环境中硝酸盐（NO）水平的升高可能对人类健康有害。在此，我们报告了一种基于混合材料的比色/发光传感器技术，该技术强大、经济高效且可扩展，用于快速、选择性、灵敏且无干扰地检测NO。这些混合材料基于负载在介孔二氧化硅上的平面正方形铂（II）盐[Pt（tpy）Cl]PF（tpy = 2,2';6',2″-三联吡啶）。在pH≤0的条件下，当铂盐暴露于NO水合阴离子时，由于PF阴离子被NO水合阴离子取代，铂盐的颜色和发光会发生显著变化。铂盐这种光物理性质的变化是由其晶格重排引起的，这导致了Pt···Pt···Pt相互作用的扩展，同时其电子结构也发生了相应变化。此外，将该材料掺入介孔二氧化硅中可增加表面积并提高检测灵敏度。实现了0.05 mM（3.1 ppm）的NO检测限，该检测限远低于美国环境保护局设定的0.16 mM（10 ppm）的环境水质限值。在存在其他干扰阴离子的情况下，混合材料的比色/发光对NO水合阴离子具有高度选择性，这表明该材料是在无需分离、浓缩或其他预处理步骤的情况下对实际样品中的NO进行快速检测和定量的有前途的候选材料。
