Center for Environmental Systems , Stevens Institute of Technology , Hoboken , New Jersey 07030 , United States.
State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences , Chinese Academy of Sciences , Beijing 100085 , China.
Environ Sci Technol. 2018 Jul 3;52(13):7343-7350. doi: 10.1021/acs.est.8b01845. Epub 2018 Jun 12.
This study revealed the effect of As on the formation and dissolution of iron (hydr)oxides and its further impact on the As removal efficacy of FeCl treatment. Adding 6.7 mg/L FeCl into 325 μg/L As solution (coprecipitation) resulted in more As removal (99% As(V) and 75% As(III)) at 2 min than adding As into aged FeCl solution (preaged, 52-87% As(V) and 7-42% As(III)) at pH 7. However, soluble As gradually increased in the coprecipitation system and decreased in the preaged system to give similar concentrations during 800 h aging. The particle size of the iron (hydr)oxides increased more slowly in the coprecipitation than in the preaged systems. These results suggest the rapid adsorption of As on Fe polymer during the initial polymerization process, which delays the growth of iron (hydr)oxides. Thermodynamically, quantum chemical calculations implied that iron ions adsorption on iron (hydr)oxide polymer was more stable than As adsorption, which is the main driving force for the As release during aging process. This study improved our understanding of the kinetic and thermodynamic processes of As adsorption and iron (hydr)oxide precipitation in the coprecipitation treatment of As, and the potential for As release during aging of sludge generated in the treatment.
本研究揭示了砷对铁(氢)氧化物形成和溶解的影响,以及其对 FeCl 处理去除砷效果的进一步影响。在 pH 值为 7 时,将 6.7mg/L 的 FeCl 添加到 325μg/L 的 As 溶液中(共沉淀),在 2 分钟内的 As 去除率(99%的 As(V)和 75%的 As(III))高于将 As 加入老化的 FeCl 溶液中(预老化,52-87%的 As(V)和 7-42%的 As(III))。然而,在 800 小时的老化过程中,共沉淀系统中的可溶性 As 逐渐增加,而预老化系统中的可溶性 As 逐渐减少,最终两者的浓度趋于相同。共沉淀系统中铁(氢)氧化物的粒径增长速度比预老化系统慢。这些结果表明,在初始聚合过程中,As 迅速吸附在 Fe 聚合物上,从而延迟了铁(氢)氧化物的生长。从热力学角度来看,量子化学计算表明,铁离子在铁(氢)氧化物聚合物上的吸附比 As 的吸附更稳定,这是老化过程中 As 释放的主要驱动力。本研究提高了我们对共沉淀处理砷过程中 As 吸附和铁(氢)氧化物沉淀动力学和热力学过程的认识,以及在处理过程中产生的污泥老化过程中 As 释放的潜力。