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羟胺促进 HO/土壤体系中三价铁还原对苯酚的降解。

Hydroxylamine promoted Fe(III) reduction in HO/soil systems for phenol degradation.

机构信息

State Key Laboratory of Biogeology and Environmental Geology, China University of Geosciences, 68 Jincheng Street, Wuhan, 430078, People's Republic of China.

Hubei Key Laboratory of Environmental and Health Effects of Persistent Toxic Substances, School of Environment and Health, Jianghan University, Wuhan, 430056, People's Republic of China.

出版信息

Environ Sci Pollut Res Int. 2022 Apr;29(20):30285-30296. doi: 10.1007/s11356-021-18345-x. Epub 2022 Jan 8.

Abstract

Production of hydroxyl radicals (•OH) upon the oxidation of solid Fe(II) by O or HO in soils and sediments has been confirmed, which benefits in situ remediation of contaminants. However, Fe(III) reduction by HO is rate-limiting. Accelerating the Fe(III)/Fe(II) cycle could improve the efficiency of remediation. This study intended to use hydroxylamine to promote Fe(III)/Fe(II) cycle during 100 g/L soil oxidation by HO for phenol degradation. The removal of phenol was 76% in 3 h during soil oxidation with 1 mM HO in the presence of 1 mM hydroxylamine but was negligible in the absence of hydroxylamine. Fe(III) in the soil was reduced to 0.21 mM Fe(II) by 1 mM hydroxylamine in 30 min. The accelerated cycle of Fe(III)/Fe(II) in the soil by hydroxylamine could effectively decompose HO to produced •OH, which was responsible for the effective enhancement of phenol degradation during soil oxidation. Under the conditions of 1 mM HO and 100 g/L soil, the pseudo-first-order kinetic constant of phenol degradation increased proportionally from 0.0453 to 0.0844 min with the increase of hydroxylamine concentrations from 0.5 to 1 mM. The kinetic constant also increased from 0.0041 to 0.0111 min with HO concentration increased from 0.5 to 2 mM, while it decreased from 0.0100 to 0.0051 min with soil dosage increased from 20 to 200 g/L. In addition, column experiments showed that phenol (10 mg/L) degradation ratio kept at about 48.7% with feeding 2 mM hydroxylamine and 2 mM HO at 0.025 PV/min. Column experiments suggested an optional application of hydroxylamine and HO for in situ remediation. The output of this study provides guidance and optional strategies to enhance contaminant degradation during soil oxidation.

摘要

在土壤和沉积物中,O 或 HO 氧化固体 Fe(II)会产生羟基自由基(•OH),这有利于污染物的原位修复。然而,HO 还原 Fe(III)是限速步骤。加速 Fe(III)/Fe(II)循环可以提高修复效率。本研究旨在使用羟胺在 HO 氧化 100g/L 土壤时促进 Fe(III)/Fe(II)循环,以降解苯酚。在有 1mM 羟胺存在的情况下,HO 氧化 3 小时内可去除 76%的苯酚,而无羟胺时则可忽略不计。在 30 分钟内,1mM 羟胺将土壤中的 Fe(III)还原为 0.21mM Fe(II)。羟胺可加速土壤中 Fe(III)/Fe(II)的循环,有效地将 HO 分解为•OH,这是 HO 氧化过程中有效增强苯酚降解的原因。在 1mM HO 和 100g/L 土壤的条件下,随着羟胺浓度从 0.5mM 增加到 1mM,苯酚降解的拟一级动力学常数从 0.0453 增加到 0.0844min'。随着 HO 浓度从 0.5mM 增加到 2mM,动力学常数也从 0.0041 增加到 0.0111min',而随着土壤用量从 20g/L 增加到 200g/L,动力学常数从 0.0100 降低到 0.0051min'。此外,柱实验表明,在以 0.025PV/min 进料 2mM 羟胺和 2mM HO 的情况下,苯酚(10mg/L)的降解率保持在约 48.7%。柱实验表明,羟胺和 HO 可用于原位修复。本研究的结果为提高土壤氧化过程中污染物降解提供了指导和可选策略。

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