Critical roles of low-molecular-weight organic acid in enhancing hydroxyl radical production by ferrous oxidation on γ-Al2O3 mineral surface

IF 11.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Water Research Pub Date : 2024-07-05 DOI:10.1016/j.watres.2024.122052

Nihong Wen , Jinsong Liu , Wenxiu Qin , Xiaolei Wang , Changyin Zhu , Dongmei Zhou

{"title":"Critical roles of low-molecular-weight organic acid in enhancing hydroxyl radical production by ferrous oxidation on γ-Al2O3 mineral surface","authors":"Nihong Wen , Jinsong Liu , Wenxiu Qin , Xiaolei Wang , Changyin Zhu , Dongmei Zhou","doi":"10.1016/j.watres.2024.122052","DOIUrl":null,"url":null,"abstract":"<div>Recognizing the pervasive presence of alumina minerals and low-molecular-weight organic acids (LMWOAs) in the environment, this study addressed the gap in the interaction mechanisms within the ternary system involving these two components and Fe(II). Specifically, the impacts of LMWOAs on hydroxyl radicals (•OH) production and iron species transformation during Fe(II) oxidation on γ-Al2O3 mineral surface were examined. Results demonstrated that adding 0.5 mM oxalate (OA) or citrate (CA) to the γ-Al2O3/Fe(II) system (28.1 μM) significantly enhanced •OH production by 1.9-fold (51.9 μM) and 1.3-fold (36.2 μM), respectively, whereas succinate (SA) exhibited limited effect (30.7 μM). Raising OA concentration to 5 mM further promoted •OH yield to 125.0 μM after 24 h. Deeper analysis revealed that CA facilitated the dissolution of adsorbed Fe(II) and its subsequent oxygenation by O2 through both one- and two-electron transfer mechanisms, whereas OA enhanced the adsorption of dissolved Fe(II) and more efficient two-electron transfer for H2O2 production. Additionally, LMWOAs presence favored the formation of iron minerals with poor crystallinity like ferrihydrite and lepidocrocite rather than well-crystallized forms such as goethite. The distinct impacts of various LMWOAs on Fe(II) oxidation and •OH generation underscore their unique roles in the redox processes at mineral surface, consequently modulating the environmental fate of prototypical pollutants like phenol.</div>","PeriodicalId":443,"journal":{"name":"Water Research","volume":null,"pages":null},"PeriodicalIF":11.4000,"publicationDate":"2024-07-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Water Research","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0043135424009527","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}

引用次数: 0

Abstract

Recognizing the pervasive presence of alumina minerals and low-molecular-weight organic acids (LMWOAs) in the environment, this study addressed the gap in the interaction mechanisms within the ternary system involving these two components and Fe(II). Specifically, the impacts of LMWOAs on hydroxyl radicals (•OH) production and iron species transformation during Fe(II) oxidation on γ-Al₂O₃ mineral surface were examined. Results demonstrated that adding 0.5 mM oxalate (OA) or citrate (CA) to the γ-Al₂O₃/Fe(II) system (28.1 μM) significantly enhanced •OH production by 1.9-fold (51.9 μM) and 1.3-fold (36.2 μM), respectively, whereas succinate (SA) exhibited limited effect (30.7 μM). Raising OA concentration to 5 mM further promoted •OH yield to 125.0 μM after 24 h. Deeper analysis revealed that CA facilitated the dissolution of adsorbed Fe(II) and its subsequent oxygenation by O₂ through both one- and two-electron transfer mechanisms, whereas OA enhanced the adsorption of dissolved Fe(II) and more efficient two-electron transfer for H₂O₂ production. Additionally, LMWOAs presence favored the formation of iron minerals with poor crystallinity like ferrihydrite and lepidocrocite rather than well-crystallized forms such as goethite. The distinct impacts of various LMWOAs on Fe(II) oxidation and •OH generation underscore their unique roles in the redox processes at mineral surface, consequently modulating the environmental fate of prototypical pollutants like phenol.

Abstract Image

查看原文

微信好友朋友圈 QQ好友复制链接

本刊更多论文

低分子量有机酸在促进γ-Al2O3 矿物表面亚铁氧化作用产生羟基自由基方面的关键作用

认识到氧化铝矿物和低分子量有机酸（LMWOAs）在环境中的普遍存在，本研究解决了涉及这两种成分和铁（II）的三元系统中相互作用机制的空白。具体来说，研究了 LMWOAs 对羟基自由基 (-OH) 生成的影响以及铁（II）在 -AlO 矿物表面氧化过程中铁物种转化的影响。结果表明，在-AlO/Fe(II)体系中加入 0.5 mM 草酸盐（OA）或柠檬酸盐（CA）（28.1 μM）可显著提高-OH 的产生，分别提高 1.9 倍（51.9 μM）和 1.3 倍（36.2 μM），而琥珀酸盐（SA）的影响有限（30.7 μM）。更深入的分析表明，CA 通过单电子转移和双电子转移机制促进了吸附的铁（II）的溶解及其随后被 O 氧化，而 OA 则增强了溶解的铁（II）的吸附和更有效的双电子转移以产生 HO。此外，LMWOAs 的存在有利于形成结晶度较低的铁矿物，如铁水石和鳞片铁矿，而不是结晶度较高的矿物，如鹅膏石。各种 LMWOAs 对铁（II）氧化和 -OH 生成的不同影响强调了它们在矿物表面氧化还原过程中的独特作用，从而调节了苯酚等原型污染物的环境归宿。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文去求助

来源期刊

Water Research 环境科学-工程：环境

CiteScore

20.80

自引率

9.40%

发文量

1307

审稿时长

38 days

期刊介绍： Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.