Kinetics and Mechanism Investigation of Selective Arsenite Oxidation by Reactive Iodine Species in Hydrogen Peroxide and Iodide (H2O2/I–) System,ACS ES&T Water

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Kinetics and Mechanism Investigation of Selective Arsenite Oxidation by Reactive Iodine Species in Hydrogen Peroxide and Iodide (H2O2/I–) System
ACS ES&T Water ( IF 4.8 ) Pub Date : 2021-06-02 , DOI: 10.1021/acsestwater.1c00062
Zhihao Chen ₁ , Jingyi Li _{1,

2} , Kok Yuen Koh _{1,

2} , Zhongrong Du _{1,

2} , Choon Nam Ong _{1,

3} , J. Paul Chen _{1,

2}

Affiliation

Pretreatment of arsenite (As(III)) to arsenate (As(V)) is crucial in remediation of As(III)-contaminated waterbodies. Hydroxyl or sulfate radicals-based advanced oxidation processes are effective; however, the efficiency becomes low as radicals can be quenched by coexisting matters besides As(III). Both I^– and As(III) coexist in several types of contaminated water such as shale gas flowback water. Herein, we proposed using H₂O₂ to react with I^– so as to generate reactive iodine species (RIS) for effective oxidation of As(III). The presence of commonly existing anions, methanol, tert-butanol, 2-propanol, formic acid, humic acid, phenol, and benzoquinone did not affect the oxidation performance. Chromate, Cu²⁺ or divalent/trivalent irons would enhance the oxidation. Only hydroquinone (>0.3 mM) had an inhibition effect on the oxidation. Unlike peroxymonosulfate and peroxydisulfate that are reactive to Cl^– or Br^–, H₂O₂ only showed a solely selective reactivity for the I^– to form the RIS. Our experimental and kinetic simulation results confirmed the most significant reaction pathway and suggested that I₂ and I₃^– were the main responsible intermediates. Our study demonstrated that the RIS possessed a higher selectivity to As(III) compared with other coexisting matters. Therefore, the application of RIS is very promising in the redox conversion mediation.

中文翻译：

过氧化氢和碘化物（H ₂ O ₂ /I ^–）体系中活性碘选择性氧化亚砷酸盐的动力学和机理研究

将亚砷酸盐 (As(III)) 预处理为砷酸盐 (As(V)) 对于修复受 As(III) 污染的水体至关重要。基于羟基或硫酸根的高级氧化工艺是有效的；然而，效率变低，因为自由基可以被除 As(III) 以外的共存物质淬灭。I ^-和 As(III) 共存于多种类型的污染水中，例如页岩气返排水。在此，我们提出了使用H ₂ ö ₂与我反应^-从而产生反应性的碘物质（RIS）对As（III）的有效氧化。常见阴离子、甲醇、叔丁醇、2-丙醇、甲酸、腐植酸、苯酚和苯醌的存在不影响氧化性能。铬酸盐，Cu ²⁺或二价/三价铁会增强氧化。只有对苯二酚 (>0.3 mM) 对氧化有抑制作用。与对 Cl ^-或 Br ^-具有反应性的过硫酸盐和过硫酸盐不同，H ₂ O ₂仅对 I ^-显示出选择性反应性，以形成 RIS。我们的实验和动力学模拟结果证实了最重要的反应途径，并表明 I ₂和 I ₃^–是主要负责的中间体。我们的研究表明，与其他共存物质相比，RIS 对 As(III) 具有更高的选择性。因此，RIS在氧化还原转化介导方面的应用前景广阔。

更新日期：2021-06-11

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