Yantasee Wassana, Fryxell Glen E, Lin Yuehe
Pacific Northwest National Laboratory, Richland, WA 99352, USA.
Analyst. 2006 Dec;131(12):1342-6. doi: 10.1039/b609211j. Epub 2006 Oct 11.
Mercury-free sensors for europium (Eu(3+)) assay based on the chemical modification of screen-printed carbon electrodes (SPCEs) with self-assembled salicylamide on mesoporous silica (Sal-SAMMS) have been developed. The preconcentration of Eu(3+) at SAMMS-based sensors utilizes the binding affinity of the salicylamide and Eu(3+), accomplished at open circuit potential without electrolyte and solution de-gassing. Optimal Eu detection was obtained after 3-5 min preconcentration in Eu solution (pH 2-6), electrolysis at -0.9 V for 60 s in a new medium (0.1-0.2 M NH(4)Cl, pH 3.5), followed by a square-wave voltammetric detection of Eu in the same electrolyte. Attributed to the strong covalent bonding of the functional groups on mesoporous silica and silane cross-linking, the SAMMS-modified SPCEs with a built-in 3-electrode system can be re-used for tens of measurements with minimal degradation, enabling the establishment of the calibration curve and lowering the costs. A linear calibration curve was found in the range of 75 to at least 500 ppb Eu(3+) after 5 min preconcentration. The experimental detection limit was 10 ppb after 10 min preconcentration, which can be improved with increased preconcentration time. Reproducibility (% RSD) of 100 ppb Eu(2+) was 10% for a single sensor and 10% for 5 sensors, which can be improved through the precision of sensor manufacturing, in which SAMMS modification can be made in-situ.
基于介孔二氧化硅上自组装水杨酰胺(Sal-SAMMS)对丝网印刷碳电极(SPCEs)进行化学修饰的无汞铕(Eu(3+))检测传感器已被开发出来。基于SAMMS的传感器对Eu(3+)的预富集利用了水杨酰胺与Eu(3+)的结合亲和力,在无电解质且溶液无需脱气的开路电位下即可完成。在Eu溶液(pH 2 - 6)中预富集3 - 5分钟后,在新介质(0.1 - 0.2 M NH(4)Cl,pH 3.5)中于-0.9 V电解60秒,然后在同一电解质中对方波伏安法检测Eu,可实现Eu的最佳检测。由于介孔二氧化硅上官能团的强共价键合和硅烷交联,带有内置三电极系统的SAMMS修饰的SPCEs可重复使用数十次且降解极小,能够建立校准曲线并降低成本。在预富集5分钟后,发现Eu(3+)在75至至少500 ppb范围内呈线性校准曲线。预富集10分钟后的实验检测限为10 ppb,随着预富集时间增加可进一步提高。对于100 ppb Eu(2+),单个传感器的重现性(% RSD)为10%,5个传感器的重现性为10%,可通过提高传感器制造精度来改善,其中SAMMS修饰可原位进行。