Liu Fu, Yang Weimin, Li Wenwen, Zhao Guang-Chao
School of Ecology and Environment, Anhui Normal University, Wuhu 241000, China.
ACS Omega. 2021 Jan 6;6(2):1477-1487. doi: 10.1021/acsomega.0c05203. eCollection 2021 Jan 19.
The major problem in arsenic (As(III)) removal using adsorbents is that the method is time-consuming and inefficient owing to the fact that most of the adsorbents are more effective for As(V). Herein, we report a new discovery regarding the significant simultaneous oxidation and sequestration of As(III) by a heterogeneous catalytic process of copper aluminate (CuAlO) coupled with peroxymonosulfate (PMS). Oxidation and adsorption promote each other. With the help of the active radicals, the As(III) removal efficiency can be increased from 59.4 to 99.2% in the presence of low concentrations of PMS (50 μM) and CuAlO (300 mg/L) in solution. CuAlO/PMS can work effectively in a wide pH range (3.0-9.0). Other substances, such as nitrate, sulfate, chloride, carbonate, and humic acid, exert an insignificant effect on As(III) removal. Based on X-ray photoelectron spectroscopy (XPS) analysis, the exposed reductive copper active sites might drive the redox reaction of Cu(II)/Cu(I), which plays a key role in the decomposition of PMS and the oxidation of As(III). The exhausted CuAlO could be refreshed for cycling runs with insignificant capacity loss by the combined regeneration strategy because of the stable spinel structure. According to all results, the CuAlO/PMS with favorable oxidation ability and stability could be employed as a promising candidate in real As(III)-contaminated groundwater treatment.
使用吸附剂去除砷(As(III))的主要问题在于,由于大多数吸附剂对As(V)更有效,该方法既耗时又低效。在此,我们报告一项关于通过铝酸铜(CuAlO)与过一硫酸盐(PMS)的非均相催化过程实现As(III)显著同步氧化和螯合的新发现。氧化和吸附相互促进。在溶液中存在低浓度PMS(50 μM)和CuAlO(300 mg/L)的情况下,借助活性自由基,As(III)的去除效率可从59.4%提高到99.2%。CuAlO/PMS能在较宽的pH范围(3.0 - 9.0)内有效发挥作用。其他物质,如硝酸盐、硫酸盐、氯化物、碳酸盐和腐殖酸,对As(III)的去除影响不大。基于X射线光电子能谱(XPS)分析,暴露的还原性铜活性位点可能驱动Cu(II)/Cu(I)的氧化还原反应,这在PMS的分解和As(III)的氧化中起关键作用。由于尖晶石结构稳定,通过联合再生策略,耗尽的CuAlO可以进行循环运行,且容量损失不显著。根据所有结果,具有良好氧化能力和稳定性的CuAlO/PMS有望成为实际受As(III)污染地下水处理的候选材料。