Liu Lihu, Zhang Mingzhe, Suib Steven L, Qiu Guohong
Key Laboratory of Arable Land Conservation (Middle and Lower Reaches of Yangtse River), Ministry of Agriculture and Rural Affairs, Hubei Key Laboratory of Soil Environment and Pollution Remediation, College of Resources and Environment, Interdisciplinary Sciences Institute, Huazhong Agricultural University, Wuhan, 430070 Hubei Province, China; Shenzhen Branch, Guangdong Laboratory for Lingnan Modern Agriculture, Genome Analysis Laboratory of the Ministry of Agriculture, Agricultural Genomics Institute at Shenzhen, Chinese Academy of Agricultural Sciences, Shenzhen, China.
Department of Chemistry, University of Connecticut, Storrs, Connecticut 06269-3060, USA.
Water Res. 2022 Nov 1;226:119297. doi: 10.1016/j.watres.2022.119297. Epub 2022 Oct 26.
Fe-Mn composite oxide (FMO) is widely applied to the oxidation and removal of As(III) from water. However, As(III) can directly reduce manganese oxides, decreasing the oxidation capacity or reusability and thereby greatly limiting the applicability of FMO. Here, the oxidation capacity and reusability of FMO for As(III) were efficiently improved by light radiation, and the effect of typical coexisting ions (SO and Ca) on the removal of As(III) was also studied. O produced from excited manganese oxide and ligand-to-metal charge transfer in iron oxide-As(III) complex enhanced As(III) oxidation and removal under light radiation. At an initial As(III) concentration of 1000 μg L, the total As concentration was respectively decreased to 11.5, 1.5 and 4.4 μg L under darkness, UV light and sunlight at 180 min, and could be reduced to below the guideline limitation of drinking water (10 μg L) within 40 and 60 min under UV light and sunlight, respectively. SO exhibited negligible effect on As removal efficiency because FMO had obviously lower adsorption capacity and selectivity for SO than for As(V). The adsorption of coexisting Ca on manganese oxide decreased the negative charge on the FMO surface, thereby improving As(III) adsorption and oxidation. FMO exhibited excellent reusability, and a total As removal efficiency of 99.1% was still maintained after five cycles of an adsorption-desorption process under UV light. This work elucidates the photochemical oxidation and removal mechanism of FMO for As(III), and proposes a low-cost and efficient method for the detoxification of As(III)-contaminated drinking water.
铁锰复合氧化物(FMO)被广泛应用于水中As(III)的氧化和去除。然而,As(III)可直接还原锰氧化物,降低其氧化能力或可重复使用性,从而极大地限制了FMO的适用性。在此,通过光辐射有效提高了FMO对As(III)的氧化能力和可重复使用性,并研究了典型共存离子(SO和Ca)对As(III)去除的影响。激发态锰氧化物产生的O以及氧化铁-As(III)络合物中的配体-金属电荷转移增强了光辐射下As(III)的氧化和去除。在初始As(III)浓度为1000 μg/L时,在黑暗、紫外光和太阳光条件下180分钟后,总砷浓度分别降至11.5、1.5和4.4 μg/L,在紫外光和太阳光下分别在40和60分钟内可降至饮用水指导限值(10 μg/L)以下。SO对As去除效率的影响可忽略不计,因为FMO对SO的吸附容量和选择性明显低于对As(V)的。共存的Ca在锰氧化物上的吸附降低了FMO表面的负电荷,从而提高了As(III)的吸附和氧化。FMO表现出优异的可重复使用性,在紫外光下经过五个吸附-解吸循环后,总As去除效率仍保持在99.1%。这项工作阐明了FMO对As(III)的光化学氧化和去除机制,并提出了一种低成本、高效的方法用于As(III)污染饮用水的解毒。