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利用 CuFe2O4 活化过一硫酸盐过程同时去除对氨基苯砷酸和释放的无机砷形态。

Simultaneous removal of para-arsanilic acid and the released inorganic arsenic species by CuFe2O4 activated peroxymonosulfate process.

机构信息

College of Civil Engineering, Zhejiang University of Technology, Hangzhou 310023, China.

College of Civil Engineering, Zhejiang University of Technology, Hangzhou 310023, China.

出版信息

Sci Total Environ. 2020 Nov 10;742:140587. doi: 10.1016/j.scitotenv.2020.140587. Epub 2020 Jun 29.

Abstract

para-arsanilic acid (p-ASA), as a major phenylarsonic feed additive, was used annually in many countries. Once it enters the water environment, p-ASA would be transformed into hypertoxic inorganic arsenic species, causing severe arsenic pollution. In this study, magnetic copper ferrite (CuFeO) was applied to activate peroxymonosulfate (PMS) for p-ASA removal and synchronous control of the released inorganic arsenic species. Results showed that CuFeO/PMS system presented favorable oxidation ability and close to 85% of 10 mg/L p-ASA was eliminated under the condition of simultaneous dosing 0.2 g/L CuFeO and 1 mM PMS. The rapid decomposition of p-ASA resulted from homogeneous PMS oxidation and the attack of reactive oxygen species (i.e., SO, HO and O), which was involved the heterogeneous PMS activation through the cycles between Fe(II)/Fe(III) and Cu(II)/Cu(I). Meanwhile, the released inorganic arsenic species during p-ASA degradation were found to be controllable via the adsorption on CuFeO surface and metal hydroxyl groups played the crucial role. CuFeO/PMS system exhibited the stable and efficient performance within the broad range of pH 3.0-11.0. The existence of common anions (Cl, NO, HCO, SO) and humic acid presented the slight inhibition for p-ASA degradation. The reduction of initial p-ASA concentration favored the p-ASA removal. Besides, the catalyst retained a favorable reactivity and stability even after four successive cycles and almost no metal leaching was observed. The rational degradation pathway was mainly involved in the cleavage of AsC bond, oxidation of amino group, substitution and oxidation of hydroxyl group. The transformation of arsenic species could be divided into the release of inorganic arsenic species, the oxidation of As(III) into As(V) and the adsorption of As(V) by CuFeO.

摘要

对氨基苯胂酸(p-ASA)作为一种主要的苯胂酸饲料添加剂,在许多国家被广泛应用。一旦进入水环境,p-ASA 将被转化为剧毒的无机砷物种,造成严重的砷污染。在本研究中,磁性铜铁氧体(CuFeO)被用于激活过一硫酸盐(PMS)以去除 p-ASA,并同步控制释放的无机砷物种。结果表明,在同时投加 0.2 g/L CuFeO 和 1 mM PMS 的条件下,CuFeO/PMS 体系具有良好的氧化能力,可去除 85%以上的 10 mg/L p-ASA。p-ASA 的快速降解归因于均相 PMS 氧化和活性氧物种(即 SO、HO 和 O)的攻击,这涉及通过 Fe(II)/Fe(III)和 Cu(II)/Cu(I)之间的循环实现异相 PMS 活化。同时,在 p-ASA 降解过程中释放的无机砷物种可以通过 CuFeO 表面的吸附得到控制,金属羟基基团起着关键作用。CuFeO/PMS 体系在 pH 3.0-11.0 的较宽范围内表现出稳定高效的性能。常见阴离子(Cl、NO、HCO、SO)和腐殖酸的存在对 p-ASA 降解的抑制作用较小。初始 p-ASA 浓度的降低有利于 p-ASA 的去除。此外,即使经过四个连续循环,催化剂仍保持良好的反应活性和稳定性,几乎没有金属浸出。合理的降解途径主要涉及 AsC 键的断裂、氨基的氧化、羟基的取代和氧化。砷物种的转化可分为无机砷物种的释放、As(III)氧化为 As(V)以及 As(V)被 CuFeO 吸附。

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