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Study of Hypochlorite Reduction Related to the Sodium Chlorate Process

机译：与氯酸钠法相关的次氯酸盐还原反应的研究

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Reduction of hypochlorite is the most important side reaction in the sodium chlorate reactor leading to high energy losses. Today chromate is added to the reactor solution to minimize the hypochlorite reduction but a replacement is necessary due to health and environmental risks with chromate. In order to understand the effect of different substrates on the hypochlorite reduction, alpha-FeOOH, gamma-FeOOH, Cr2O3 and CrOH3 were electrodeposited on titanium and subjected to electrochemical investigations. These substances are commonly found on cathodes in the chlorate process and can serve as model substances for the experimental investigation. The mechanism of hypochlorite reduction was also studied using DFT calculations in which the reaction at Fe(III) and Cr(III) surface sites were considered in order to single out the electrocatalytic properties. The experimental results clearly demonstrated that the chromium films completely block the reduction of hypochlorite, while for the iron oxyhydroxides the process can readily occur. Since the electrocatalytic properties per se were shown by the DFT calculations to be very similar for Fe(III) and Cr(III) sites in the oxide matrix, other explanations for the blocking ability of chromium films are addressed and discussed in the context of surface charging, reduction of anions and conduction in the deposited films. The main conclusion is that the combined effect of electronic properties and reduction of negatively charged ions can explain the reduction kinetics of hypochlorite and the effect of chromate in the chlorate process.
机译：次氯酸盐的还原是氯酸钠反应器中最重要的副反应，导致高能量损失。如今，将铬酸盐添加到反应器溶液中可最大程度地减少次氯酸盐的还原，但是由于铬酸盐的健康和环境风险，因此有必要进行替代。为了了解不同基质对次氯酸盐还原的影响，将α-FeO​​OH，γ-FeOOH，Cr2O3和CrOH3电沉积在钛上并进行电化学研究。这些物质通常在氯酸盐工艺中的阴极上发现，可以用作实验研究的模型物质。还使用DFT计算研究了次氯酸盐还原的机理，在DFT计算中考虑了在Fe（III）和Cr（III）表面位的反应，以找出电催化性能。实验结果清楚地表明，铬膜完全阻止了次氯酸盐的还原，而对于羟基氧化铁，该过程很容易发生。由于DFT计算表明，对于氧化物基体中的Fe（III）和Cr（III）部位，其本身的电催化性能非常相似，因此在表面情况下讨论并讨论了铬膜阻挡能力的其他解释。带电，阴离子减少和沉积膜中的导电。主要结论是，电子性质与带负电离子的还原的综合作用可以解释次氯酸盐的还原动力学以及氯酸盐在氯酸盐过程中的作用。

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