UNSW Water Research Centre, School of Civil and Environmental Engineering , The University of New South Wales , Sydney , New South Wales 2052 , Australia.
Environ Sci Technol. 2019 Aug 20;53(16):9715-9724. doi: 10.1021/acs.est.9b01762. Epub 2019 Aug 5.
Constrained by low energy efficiency and ineffectiveness in As(III) removal under circumneutral pH conditions by many exsiting technologies, As(III) removal has become an issue. In this work we present proof of concept of a modified double potential step chronoamperometry (DPSC) method of As(III) oxidation and concomitant As(V) electro-sorption from aqueous solution. Results show that in situ anodic As(III) oxidation, As(V) electro-sorption, and As(V) electro-desorption are affected by aqueous pH with high oxidation and sorption/desorption rates observed at the elevated pH. We particularly show that effective As(III) oxidation and concomitant As(V) adsorption are related to (i) the rapid oxidation of the deprotonated species compared to the protonated species and (ii) stronger electrochemical interaction between the multicharged As(V) species and the electrodes. At 1.2 V and an electric energy consumption of 0.06 kWh m, the total As concentration can be reduced from 150 to 15 μg L using an electrochemical cell with electrode area of 10 × 8 cm and electro-sorption time of 120 min. On the basis of the experimental results, we have developed a mathematical model to describe the kinetics and mechanism of arsenic removal by the modified DPSC method with this model of use in predicting, and potentially optimizing, process performance under various conditions.
受许多现有技术在中性 pH 条件下低能量效率和去除 As(III)效果不佳的限制,去除 As(III)已成为一个问题。在这项工作中,我们提出了一种改进的双电位阶跃计时安培法(DPSC)的概念验证,用于从水溶液中氧化 As(III)并同时电吸附 As(V)。结果表明,溶液 pH 会影响原位阳极氧化 As(III)、电吸附 As(V)和电脱附 As(V),在升高的 pH 值下观察到高氧化和吸附/脱附速率。我们特别表明,有效的 As(III)氧化和同时的 As(V)吸附与(i)与质子化物种相比,去质子化物种的快速氧化和(ii)多电荷 As(V)物种与电极之间更强的电化学相互作用有关。在 1.2 V 和 0.06 kWh m 的电能消耗下,使用电极面积为 10 × 8 cm 的电化学电池和 120 min 的电吸附时间,可将总砷浓度从 150 μg L 降低至 15 μg L。基于实验结果,我们开发了一种数学模型来描述通过改进的 DPSC 方法去除砷的动力学和机制,该模型可用于预测和潜在优化各种条件下的工艺性能。