首页|水铁矿表面介导亚铁有氧氧化产生羟基自由基性能及其应用

水铁矿表面介导亚铁有氧氧化产生羟基自由基性能及其应用

扫码查看
采用外源添加Fe(Ⅱ)和As(Ⅲ)的反应体系,重点研究水铁矿表面介导活性氧物种(ROS)的产生及其对As(Ⅲ)氧化转化的增效机理.XRD、ESR以及XPS等分析结果均表明:水铁矿/Fe(Ⅱ)体系在弱酸性pH条件下氧化产生的ROS包含有羟自由基.OH、单线态氧1O2和超氧自由基·O2-,且产.OH的类芬顿反应是一个单电子传递的过程.水铁矿/Fe(Ⅱ)体系氧化反应120 min时可生成约364.82 µmol/L的H2O2,O2的存在高度决定了 H2O2的生成.水铁矿/Fe(Ⅱ)体系中的.OH累积浓度与Fe(Ⅱ)氧化的量成正比,pH为6的弱酸性条件更有利于水铁矿/Fe(Ⅱ)体系氧化产.OH,此时体系产生的·OH累积浓度约为30.69 μmol/L.As(Ⅲ)被·OH等ROS氧化主要发生在矿物固体表面,Fe(Ⅱ)的存在有利于该体系氧化As(Ⅲ)形成As(V),但由于存在竞争吸附,因而可能不利于该体系吸附As(Ⅲ)及后续的界面氧化作用.该研究将有助于丰富基于矿物表面介导的Fe(Ⅱ)反应性对砷污染环境净化耦合作用增强机制的认识,可为实际砷污染土壤环境修复提供实验与理论依据.
Performance of Goethite Surface-mediated Ferrous Iron Aerobic Oxidation to Generate Hydroxyl Radicals and Its Application
By externally adding Fe(Ⅱ)and Fe(Ⅲ)to the reaction system,this study focuses on investigating the production of reactive oxygen species(ROS)mediated by the surface of goethite and its enhancement mechanism for the oxidation and transformation of As(Ⅲ).The analyses with XRD,ESR,and XPS indicated that ROS gener-ated in the oxidation of the ferrihydrite/Fe(Ⅱ)system under weakly acidic pH conditions includes hydroxyl radical·OH,singlet oxygen 1O2,and superoxide radical·O2-,while the Fenton like reaction for the·OH production is a single electron transfer process.Approximately 364.82 μmol/L H2O2 can be generated during the oxidation reaction of ferrihydrite/Fe(Ⅱ)system for 120 min,and the presence of O2 highly determined the generation of H2O2.The·OH cumulative concentration in the above ferrihydrite/Fe(Ⅱ)system is positively correlated with the amount of Fe(Ⅱ)to be oxidized.A weak weak acidic condition at pH 6 is more favorable for the ferrous oxygenation reaction system to produce OH,wherein the OH cumulative concentration is about 30.69 μmol/L.Moreover,the oxida-tion of As(Ⅲ)by ROS such as·OH species mainly occurs on mineral surfaces.The presence of Fe(Ⅱ)is condu-cive to the occurrence of As(Ⅲ)oxidation to form As(V)in the system,but due to competitive adsorption,the Fe(Ⅱ)adsorption may not be conducive to both the adsorption of As(Ⅲ)and its subsequent interfacial oxidation in the system.As a result,this study will contribute to well-understanding of the synergistic mechanism of Fe(Ⅱ)reactivity mediated by mineral surfaces coupling with the enhancement in arsenic pollution environmental purifica-tion,and thus may provide the experimental and theoretical bases for practical arsenic contaminated soil environ-mental remediation.

ferrihydriteferrous iron oxygenationhydroxyl radicalArseniteoxidative transformation

陈静、谭欣洁、杨露、吴宏海、李耀威

展开 >

华南师范大学环境学院,广州 510006

水铁矿 亚铁有氧氧化 羟自由基 三价砷 氧化转化

2024

华南师范大学学报(自然科学版)
华南师范大学

华南师范大学学报(自然科学版)

CSTPCD北大核心
影响因子:0.413
ISSN:1000-5463
年,卷(期):2024.56(5)