Department of Chemistry, National Taiwan University, 1, Section 4, Roosevelt Road, Taipei, 10617, Taiwan.
Nanoscience and Technology Program, Taiwan International Graduate Program, Academia Sinica, Taipei, 11529, Taiwan.
Anal Bioanal Chem. 2018 Jul;410(18):4555-4564. doi: 10.1007/s00216-018-1114-7. Epub 2018 Jun 4.
We have devised a unique strategy for highly sensitive, selective, and colorimetric detection of mercury based on analyte-induced enhancement of the photocatalytic activity of TiO-Au nanospheres (TiO-Au NSs) toward degradation of methylene blue (MB). Through electrostatic interactions, Au nanoparticles are attached to poly-(sodium 4-styreneulfonate)/poly(diallyldimethylammonium chloride) modified TiO nanoparticles, which then form an Au shell on each TiO core through reduction of Au with ascorbic acid. Notably, the deposition of Hg species (Hg/CHHg) onto TiO-Au NSs through strong Au-Hg aurophilic interactions speeds up catalytic degradation of MB. The first-order degradation rates of MB by TiO-Au NSs and TiO-Au-Hg NSs are 1.4 × 10 min and 2.1 × 10 min, respectively. Using a commercial absorption spectrometer, the TiO-Au NSs/MB approach provides linearity (R = 0.98) for Hg over a concentration range of 10.0 to 100.0 nM, with a limit of detection (LOD) of 1.5 nM. On the other hand, using a low-cost smartphone app that records the color changes (ΔRGB) of MB solution based on the red-blue-green (RGB) component values, the TiO-Au NSs/MB approach provides an LOD of 2.0 nM for Hg and 5.0 nM for CHHg, respectively. Furthermore, the smartphone app sensing system has been validated for the analyses of various samples, including tap water, lake water, soil, and Dorm II, showing its great potential for on-line analysis of environmental and biological samples. Graphical Abstract ᅟ.
我们设计了一种独特的策略,用于基于 TiO-Au 纳米球(TiO-Au NSs)对亚甲基蓝(MB)降解的光催化活性的分析物诱导增强,实现对汞的高灵敏度、选择性和比色检测。通过静电相互作用,将金纳米颗粒附着在聚(4-苯乙烯磺酸钠)/聚(二烯丙基二甲基氯化铵)修饰的 TiO2 纳米颗粒上,然后通过抗坏血酸还原在每个 TiO 核上形成 Au 壳。值得注意的是,Hg 物种(Hg/CHHg)通过强 Au-Hg 金键相互作用沉积在 TiO-Au NSs 上,加速了 MB 的催化降解。TiO-Au NSs 和 TiO-Au-Hg NSs 对 MB 的一阶降解速率分别为 1.4×10-1 min-1 和 2.1×10-1 min-1。使用商业吸收光谱仪,TiO-Au NSs/MB 方法在 10.0 至 100.0 nM 的浓度范围内对 Hg 提供线性(R=0.98),检测限(LOD)为 1.5 nM。另一方面,使用记录 MB 溶液颜色变化(ΔRGB)的低成本智能手机应用程序,基于红-蓝-绿(RGB)分量值,TiO-Au NSs/MB 方法分别对 Hg 和 CHHg 的检测限为 2.0 nM 和 5.0 nM。此外,智能手机应用程序传感系统已被验证用于各种样品的分析,包括自来水、湖水、土壤和 Dorm II,表明其在环境和生物样品的在线分析方面具有巨大的潜力。