4.6 Article

Arsenite removal in a goethite/oxalate system under UVA irradiation: Roles of different reactive species in acidic and neutral conditions

期刊

JOURNAL OF MOLECULAR STRUCTURE
卷 1245, 期 -, 页码 -

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ELSEVIER
DOI: 10.1016/j.molstruc.2021.131065

关键词

Arsenite; Goethite; Oxalate; Hydroxyl radical; Photo-generated hole

资金

  1. National Natural Science Foun-dation of China [21667011]
  2. Science and Technology Fund of Guizhou Province [[2018] 1078, ZK [2021] 099]
  3. construction project of Key Laboratory of State Ethnic Affairs Com-mission [91]

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This study examined arsenite (As(III)) removal in a goethite/oxalate suspension under UVA-irradiation, finding that pH, oxalate concentration, and goethite dosage significantly affected removal efficiency. Increasing pH decreased photo-oxidation efficiency but increased adsorption efficiency, while the addition of oxalate promoted As(III) removal. The use of appropriate amounts of goethite accelerated removal, with different mechanisms observed for As(III) removal under neutral and acidic conditions.
In this work, arsenite (As(III)) removal in a goethite/oxalate suspension under UVA-irradiation (lambda(max) = 365 nm) was explored under different conditions (initial pH, oxalate concentration, goethite dosage, and phosphate). SEM, EDS, FTIR, XRD and XPS were used to investigate the morphology, composition, functional groups, structure, and surface properites of goethite. The greatest efficiency of As(III) removal was 95.52% at pH 3.0, 100.0 mu g.L-1 As(III), 0.05 g.L-1 goethite, and 0.5 mmol.L-1 oxalate. The removal of As(III) in the goethite/oxalate system was strongly pH-dependent. An increase in pH was accompanied by a reduction in photo-oxidation efficiency and an increase in adsorption efficiency. Addition of appropriate amounts of oxalate can enhance As(III) removal at pH 3.0 by promoting the photo-dissolution of iron oxide. However, the addition of oxalate was detrimental to As(III) removal at pH 7.0 due to its competition for photo-generated hole (h(vb)(+)) as well as adsorption sites. Increasing dosage from 0.0 to 0.5 g.L-1 accelerated As(III) removal at both pH 3.0 and pH 7.0. ESR, radical-scavenging, and N-2-purging experiments showed that As(III) removal was mainly achieved by photo-oxidation at pH 3.0 and HO. appeared to be the primary oxidant for the As(III) oxidation, which was strongly dependent on HO2 center dot/O-2(center dot-). However, adsorption served as a major pathway and photo-oxidation played a minor role at pH 7.0. As(III) photo-oxidation was predominantly attributed to the direct reaction between As(III) and h(vb)(+) under neutral conditions. In addition, O-2 played an important role in As(III) photo-oxidation under acidic and neutral conditions. Moreover, goethite remained morphologically intact and demonstrated good reusability up to five regeneration cycles. These findings show that As(III) can be effectively removed from water containing iron oxides and carboxylic acid, which is important for the remediation of arsenic-contaminated waterbodies and wastewaters. (C) 2021 Elsevier B.V. All rights reserved.

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