腐植酸抑制针铁矿表面Fe（II）氧化过程中羟基自由基的生成

IF 8 1区环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES

Science of the Total Environment Pub Date : 2025-02-10 DOI:10.1016/j.scitotenv.2025.178581

Meiru Yin , Wentao Yu , Siyu Nie , Kun Wang , Xin Xiao , Baoliang Chen

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引用次数: 0

摘要

在缺氧-缺氧界面上，铁（II）氧化形成的羟基自由基（•OH）已被越来越多地认识到。矿物对Fe（II）的吸附改变了Fe（II）的反应活性，对Fe（II）的氧化起着重要的作用。然而，溶解有机物（DOM）对矿物吸附铁（II）氧化和•OH生成的影响尚不清楚。在此，我们研究了腐植酸（HA）对针铁矿表面吸附铁（II）氧化过程中•OH积累的影响。研究发现，与针铁矿吸附Fe（II）促进•OH生成相比，添加100-500 mg C•L−1 HA可抑制3.7% - 24.8%•OH的积累，并且•OH生成的电子利用效率从15.4%降低到11.8%。缺氧条件下的吸附实验表明，羟基磷灰石在针铁矿表面与铁（II）竞争吸附。XPS光谱分析表明，羟基磷酰胺使铁- oh表面官能团减少4.8%，从而减少针铁矿上的活性位点。伏安循环曲线表明，羟基磷灰石降低了针铁矿吸附Fe（II）的还原能力，抑制了其电导率。本研究阐明了针铁矿表面Fe（II）氧化过程中HA吸附对•OH生成的影响及其机理。

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Humic acid inhibits hydroxyl radical generation during oxygenation of Fe(II) on goethite surface

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Humic acid inhibits hydroxyl radical generation during oxygenation of Fe(II) on goethite surface

The dark formation of hydroxyl radicals (•OH) by the oxidation of Fe(II) has been increasingly recognized at anoxic–oxic interface. Minerals play significant roles on oxidation of Fe(II) owing to the adsorption changed the reactivity of Fe(II). However, the impact of dissolved organic matter (DOM) on the oxidation of mineral adsorbed Fe(II) and •OH generation remains unknown. Herein, we examined the impact of humic acid (HA) on •OH accumulation during oxygenation of goethite surface-adsorbed Fe(II). We found the addition of 100–500 mg C•L⁻¹ HA inhibited 3.7 % - 24.8 % •OH accumulation, compared to •OH generation facilitated by goethite-adsorbed Fe(II), and the electron utilization efficiency for •OH generation reduced from 15.4 % to 11.8 %. The adsorption experiment under anoxic condition showed that HA compete absorption with Fe(II) on goethite surface. XPS spectroscopy revealed that HA reduces the surface Fe-OH functional group by 4.8 %, thereby reducing the active sites on goethite. Voltammetric cycling curves demonstrated that HA decreased the reducing capacity and inhibited the electrical conductivity of the goethite-adsorbed Fe(II). This study elucidates the effects and mechanisms of HA adsorption on •OH generation during the oxygenation of Fe(II) on goethite surface.

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来源期刊

Science of the Total Environment 环境科学-环境科学

CiteScore

17.60

自引率

10.20%

发文量

8726

审稿时长

2.4 months

期刊介绍： The Science of the Total Environment is an international journal dedicated to scientific research on the environment and its interaction with humanity. It covers a wide range of disciplines and seeks to publish innovative, hypothesis-driven, and impactful research that explores the entire environment, including the atmosphere, lithosphere, hydrosphere, biosphere, and anthroposphere. The journal's updated Aims & Scope emphasizes the importance of interdisciplinary environmental research with broad impact. Priority is given to studies that advance fundamental understanding and explore the interconnectedness of multiple environmental spheres. Field studies are preferred, while laboratory experiments must demonstrate significant methodological advancements or mechanistic insights with direct relevance to the environment.