Kinetic research of scorodite formation via oxidative coprecipitation from arsenic–bearing solution

IF 6.9 2区 环境科学与生态学 Q1 ENGINEERING, CHEMICAL
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Abstract

Atmospheric oxidation is one frequently–used method to immobilize arsenic-bearing wastewater as nonhazardous scorodite. Its kinetic research is indispensable for improving synthesis on an industrial scale. In this study, the kinetic for the conversion from ionic Fe(II) and As(V) solution to scorodite was elaborately researched and discussed based on temperature–dependent experiments and software calculations. This work was divided into three parts. In experiments, scorodite synthesis was based on the optimal conditions of initial pH 2.0, 20 g/L of As, Fe/As molar ratio 1.4, O2 flow rate 0.5 L·min−1 at 95℃ for 12 h. Moreover, scorodite is developed from polymerization and oxidation determined by solution pH, residual [As] and [Fe(II)] with the precipitate phase transformation observed by X–ray diffraction and scanning electron microscope. In kinetic analysis, the activation energy of Fe(II)–As(V) polymerization and oxidation varied at 33.81–435.27 kJ·mol−1 and 52.66–599.25 kJ·mol−1, respectively, calculated from Arrhenius equation based on the established matrix equation solved by Matlab software. In synthetic improving, the whole process is comprised of atmospheric polymerization at 90 ℃ for 1.5 h followed by pressurized oxidation at 130 ℃ and PO2=1.5 MPa for 3 h as the rate constants of polymerization far outweighs that of oxidation. In general, this kinetic research is reliable and can be applied to other arsenic immobilization from arsenic–bearing solution. The improved synthesis for scorodite is more advanced in reaction duration and oxygen utilization for potential industrial application.

含砷溶液通过氧化共沉淀形成蝎尾石的动力学研究
大气氧化法是将含砷废水固定为无害菱镁矿的一种常用方法。其动力学研究对于改进工业规模的合成是不可或缺的。在本研究中,根据温度相关实验和软件计算,对离子型 Fe(II) 和 As(V) 溶液转化为蝎尾石的动力学进行了详细研究和讨论。这项工作分为三个部分。在实验中,蝎尾石的合成是在初始 pH 值为 2.0、As 为 20 g/L、Fe/As 摩尔比为 1.4、O2 流量为 0.5 L-min-1、温度为 95℃、持续 12 小时的最佳条件下进行的。此外,根据溶液 pH 值、残留[As]和[Fe(II)]来确定聚合和氧化过程中生成的蝎尾石,并通过 X 射线衍射和扫描电子显微镜观察沉淀物的相变。在动力学分析中,Fe(II)-As(V)聚合和氧化的活化能分别为 33.81-435.27 kJ-mol-1 和 52.66-599.25 kJ-mol-1。在合成改良过程中,由于聚合的速率常数远大于氧化的速率常数,整个过程包括在 90 ℃ 下常压聚合 1.5 小时,然后在 130 ℃ 和 PO2=1.5 MPa 下加压氧化 3 小时。总的来说,这项动力学研究是可靠的,可以应用于其他含砷溶液的砷固定化。改进后的蝎尾石合成法在反应持续时间和氧气利用方面更为先进,具有潜在的工业应用价值。
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来源期刊
Process Safety and Environmental Protection
Process Safety and Environmental Protection 环境科学-工程:化工
CiteScore
11.40
自引率
15.40%
发文量
929
审稿时长
8.0 months
期刊介绍: The Process Safety and Environmental Protection (PSEP) journal is a leading international publication that focuses on the publication of high-quality, original research papers in the field of engineering, specifically those related to the safety of industrial processes and environmental protection. The journal encourages submissions that present new developments in safety and environmental aspects, particularly those that show how research findings can be applied in process engineering design and practice. PSEP is particularly interested in research that brings fresh perspectives to established engineering principles, identifies unsolved problems, or suggests directions for future research. The journal also values contributions that push the boundaries of traditional engineering and welcomes multidisciplinary papers. PSEP's articles are abstracted and indexed by a range of databases and services, which helps to ensure that the journal's research is accessible and recognized in the academic and professional communities. These databases include ANTE, Chemical Abstracts, Chemical Hazards in Industry, Current Contents, Elsevier Engineering Information database, Pascal Francis, Web of Science, Scopus, Engineering Information Database EnCompass LIT (Elsevier), and INSPEC. This wide coverage facilitates the dissemination of the journal's content to a global audience interested in process safety and environmental engineering.
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