Pandey Prem C, Shukla Shubhangi, Narayan Roger J
Department of Chemistry, Indian Institute of Technology (BHU), Varanasi 221005, India.
Joint Department of Biomedical Engineering, University of North Carolina, Chapel Hill, NC 27599, USA.
Nanomaterials (Basel). 2021 Apr 28;11(5):1145. doi: 10.3390/nano11051145.
Prussian blue nanoparticles (PBN) exhibit selective fluorescence quenching behavior with heavy metal ions; in addition, they possess characteristic oxidant properties both for liquid-liquid and liquid-solid interface catalysis. Here, we propose to study the detection and efficient removal of toxic arsenic(III) species by materializing these dual functions of PBN. A sophisticated PBN-sensitized fluorometric switching system for dosage-dependent detection of As along with PBN-integrated SiO platforms as a column adsorbent for biphasic oxidation and elimination of As have been developed. Colloidal PBN were obtained by a facile two-step process involving chemical reduction in the presence of 2-(3,4-epoxycyclohexyl)ethyl trimethoxysilane (EETMSi) and cyclohexanone as reducing agents, while heterogeneous systems were formulated via EETMSi, which triggered in situ growth of PBN inside the three-dimensional framework of silica gel and silica nanoparticles (SiO). PBN-induced quenching of the emission signal was recorded with an As concentration (0.05-1.6 ppm)-dependent fluorometric titration system, owing to the potential excitation window of PBN (at 480-500 nm), which ultimately restricts the radiative energy transfer. The detection limit for this arrangement is estimated around 0.025 ppm. Furthermore, the mesoporous and macroporous PBN-integrated SiO arrangements might act as stationary phase in chromatographic studies to significantly remove As. Besides physisorption, significant electron exchange between Fe/Fe lattice points and As ions enable complete conversion to less toxic As ions with the repeated influx of mobile phase. PBN-integrated SiO matrices were successfully restored after segregating the target ions. This study indicates that PBN and PBN-integrated SiO platforms may enable straightforward and low-cost removal of arsenic from contaminated water.
普鲁士蓝纳米颗粒（PBN）对重金属离子表现出选择性荧光猝灭行为；此外，它们在液-液和液-固界面催化中均具有独特的氧化性能。在此，我们提议通过实现PBN的这些双重功能来研究有毒砷（III）物种的检测和有效去除。已开发出一种用于剂量依赖性检测砷的复杂的PBN敏化荧光开关系统，以及作为用于双相氧化和去除砷的柱吸附剂的PBN集成SiO平台。通过一种简便的两步法获得胶体PBN，该方法涉及在2-（3,4-环氧环己基）乙基三甲氧基硅烷（EETMSi）和环己酮作为还原剂的存在下进行化学还原，而异质体系则通过EETMSi配制，EETMSi触发了PBN在硅胶和二氧化硅纳米颗粒（SiO）的三维框架内原位生长。由于PBN的潜在激发窗口（在480-500nm）最终限制了辐射能量转移，因此使用砷浓度（0.05-1.6ppm）依赖性荧光滴定系统记录了PBN诱导的发射信号猝灭。这种配置的检测限估计约为0.025ppm。此外，介孔和大孔PBN集成SiO配置在色谱研究中可能用作固定相，以显著去除砷。除了物理吸附外，Fe/Fe晶格点与砷离子之间的大量电子交换能够在流动相反复流入的情况下将砷完全转化为毒性较小的砷离子。分离目标离子后，PBN集成SiO基质成功恢复。这项研究表明，PBN和PBN集成SiO平台可以实现从受污染水中直接且低成本地去除砷。
