Department of Chemical and Environmental Engineering, University of California, Riverside, CA, 92521, USA; UCR Center for Catalysis, University of California, Riverside, CA, 92521, USA.
UCR Center for Catalysis, University of California, Riverside, CA, 92521, USA; Department of Chemistry, University of California, Riverside, CA, 92521, USA.
Water Res. 2017 Jan 1;108:383-390. doi: 10.1016/j.watres.2016.11.013. Epub 2016 Nov 4.
Hexavalent chromium Cr(VI), a highly toxic oxyanion, widely occurs in drinking water supplies. This study designed and synthesized a new type of highly reductive TiO nanocrystals for photochemical Cr(VI) removal, via the thermal hydrolysis of TiCl in the presence of diethylene glycol (DEG). Surface analyses and hydroxyl radical measurements suggested that DEG was chemically bonded on TiO surface that resulted in an internal hole-scavenging effect and a high electron-releasing capacity, making it advantageous to conventional TiO materials. Upon UV irradiation, the synthesized TiO photocatalyst exhibited fast Cr(VI) reduction kinetics in diverse water chemical conditions. Fast elimination of Cr(VI) was achieved on a time scale of seconds in drinking water matrices. The removal of Cr(VI) by reductive TiO exhibited a three-stage kinetic behavior: an initial fast-reaction phase, a lag phase resulting from surface precipitation of Cr(OH) and a final reaction phase due to surface regeneration from oxidation-reduction induced ripening process. The lag phase disappeared in acidic conditions that prevented the formation of Cr(OH). The catalyst exhibited extremely high electron-releasing capacity that can be reused for multiple cycles of Cr(VI) removal in drinking water treatment.
六价铬 Cr(VI),一种毒性很高的含氧阴离子,广泛存在于饮用水供应中。本研究设计并合成了一种新型的高还原性 TiO 纳米晶体,用于光化学去除 Cr(VI),方法是在二乙二醇 (DEG) 的存在下通过 TiCl 的热水解来实现。表面分析和羟基自由基测量表明,DEG 与 TiO 表面发生化学结合,导致内部空穴清除效应和高电子释放能力,这使得它优于传统的 TiO 材料。在 UV 照射下,合成的 TiO 光催化剂在各种水化学条件下表现出快速的 Cr(VI)还原动力学。在饮用水基质中,Cr(VI)的去除在几秒钟的时间尺度内实现。还原 TiO 去除 Cr(VI)表现出三阶段动力学行为:初始快速反应阶段、由于 Cr(OH)表面沉淀导致的滞后阶段和由于氧化还原诱导熟化过程导致的表面再生的最终反应阶段。在酸性条件下,滞后阶段消失,因为这可以防止 Cr(OH)的形成。该催化剂表现出极高的电子释放能力,可在饮用水处理中重复用于多次 Cr(VI)去除循环。