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Impact of Phosphate on Ferrate Oxidation of Organic Compounds: An Underestimated Oxidant

机译：磷酸盐对高铁酸盐氧化有机化合物的影响：氧化剂被低估

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摘要

Ferrate (K2FeO4) is a powerful oxidant and up to 3 mol of electrons could be captured by 1 mol of ferrate in the theoretical conversion of Fe(VI)-Fe(V)-Fe(IV)-Fe(III). However, it is reported that the utilization efficiency of the ferrate oxidation capacity is quite low because of the rapid autodecomposition of intermediate iron species, which negatively influences the potential of ferrate on organic pollutants control. We accidentally found that for the ferrate oxidation of carbamazepine (CBZ), bisphenol S (BPS), diclofenac (DCF), and ciprofloxacin (CIP), the determined reaction rate constants were 1.7-2.4 times lower in phosphate buffer than those in borate buffer at pH 8.0. For the reaction of ferrate with 2,2'-azino-bis(3-ethylbenzothiazoline-6-sulfonate) (ABTS) at pH 7.0, the determined reaction stoichiometries were 1:1.04 in 100 mM phosphate buffer, 1:1.18 in 10 mM phosphate buffer, and 1:1.93 in 10 mM borate buffer, respectively. The oxidation ability of ferrate seems depressed in phosphate buffer. A kinetic model involving the oxidation of ABTS by Fe(VI), Fe(V) and Fe(IV) species was developed and fitted the ABTS(center dot+) formation kinetics well under different buffer conditions. The results showed that phosphate exhibited little influence on the oxidation ability of Fe(VI) and Fe(IV) species, but decreased the specific rate constants of ABTS with Fe(V) species by 1-2 orders of magnitude, resulting in the outcompeting of Fe(V) autodecomposition pathway. The complexation between phosphate anions and Fe(V) species may account for the inhibition effect of phosphate buffer. Considering that many studies regarding ferrate oxidation were carried out in phosphate buffer, the actual oxidation ability of ferrate may be underestimated.
机译：高铁酸盐（K2FeO4）是一种强氧化剂，在理论上将Fe（VI）-Fe（V）-Fe（IV）-Fe（III）转化时，1摩尔高铁酸盐可捕获多达3摩尔电子。然而，据报道，由于中间铁物种的快速自分解，高铁酸盐氧化能力的利用效率非常低，这不利地影响了高铁酸盐对有机污染物控制的潜力。我们意外地发现，对于卡马西平（CBZ），双酚S（BPS），双氯芬酸（DCF）和环丙沙星（CIP）的高铁酸盐氧化，所确定的反应速率常数在磷酸盐缓冲液中比在硼酸盐缓冲液中低1.7-2.4倍。在pH 8.0下。对于高铁酸盐与2,2'-叠氮基双（3-乙基苯并噻唑啉-6-磺酸盐）（ABTS）在pH 7.0下的反应，测定的化学计量比在100 mM磷酸盐缓冲液中为1：1.04，在10 mM中为1：1.18磷酸盐缓冲液和10 mM硼酸盐缓冲液中的1：1.93。在磷酸盐缓冲液中，高铁酸盐的氧化能力似乎降低了。建立了涉及Fe（VI），Fe（V）和Fe（IV）物种氧化ABTS的动力学模型，并在不同缓冲条件下很好地拟合了ABTS（中心点+）形成动力学。结果表明，磷酸盐对Fe（VI）和Fe（IV）物种的氧化能力几乎没有影响，但将ABTS与Fe（V）物种的比速率常数降低了1-2个数量级，从而导致了竞争。 Fe（V）自分解途径磷酸根阴离子和Fe（V）物种之间的络合可能解释了磷酸根缓冲剂的抑制作用。考虑到在磷酸盐缓冲液中进行了许多有关高铁酸盐氧化的研究，可能会低估高铁酸盐的实际氧化能力。

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  • 来源
    《Environmental Science & Technology》 |2018年第23期|13897-13907|共11页
  • 作者

    Huang Zhuang-Song; Wang Lu; Liu Yu-Lei; Jiang Jin; Xue Mang; Xu Cheng-Biao; Zhen Yu-Fei; Wang Yi-Cheng; Ma Jun;

  • 作者单位

    Dalian Polytech Univ, Sch Light Ind & Chem Engn, Dalian 116034, Peoples R China;

    Dongguan Univ Technol, Technol R&D Ctr Environm Engn, Dongguan 523808, Peoples R China;

    Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Sch Environm, Harbin 150090, Heilongjiang, Peoples R China;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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