草酸强化天然铁矿石异相光助Fenton催化降解萘酚

摘要
图/表
参考文献
相关文章 (15)

全文: PDF (1993 KB) HTML (0 KB)
输出: BibTeX | EndNote (RIS)

摘要对安徽马鞍山天然铁矿石的结构与成分进行表征分析，利用响应曲面方法箱线型设计（BBD）评估影响萘酚降解效率因素之间的交互作用，并探讨草酸强化铁矿石异相光助Fenton催化体系的机理.结果显示，马鞍山铁矿石的矿石矿物主要为磁铁矿.性能评价结果显示草酸显著提高铁矿石异相光助Fenton催化性能，萘酚去除率由40%提高至>99%.BBD设计表明影响萘酚降解的主导因素是草酸浓度，其次是H₂O₂浓度，铁矿石剂量的影响稍小，三者之间均存在交互影响.EPR结果表明草酸的引入可以显著提高体系中的CO₂^·—和O₂^·—含量.草酸强化铁矿石异相光助Fenton高效催化降解萘酚主要归因于草酸与铁矿石形成的草酸铁络合物的光分解提高体系中O₂^·—产量，另一方面光分解产物Fe （Ⅱ）加速Fenton反应产生·OH的速率.研究结果可为绿色环保水污染物控制技术研发提供指导.

	服务

	把本文推荐给朋友
	加入我的书架
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	胡彩萍
	锁进然
	丁冠涛
	徐天缘
	魏善明
	王坤

关键词 ：铁矿, 草酸, 异相Fenton, 多环芳烃, 机理

Abstract：In this study, the structure and composition of the natural iron mineral collected from Maanshan were characterized, and the box-plot design (BBD) of the response surface method was used to evaluate the influencing factors. Moreover, the mechanism of enhanced heterogeneous photo-Fenton activity by oxalate was discussed. The characterization result show that the Maanshan iron mineral is mainly magnetite. The performance evaluation results reveal that oxalate can significantly improve the heterogeneous photo-Fenton activity of the iron mineral, and the removal rate of naphthol increased from 40% to >99% after oxalate addition. The BBD design shows that the dominant factor affecting the degradation of naphthol was oxalate concentration, followed by H₂O₂ concentration. The EPR results reveal that introducing oxalate could significantly improve the generation of CO₂^·- and O₂^·-. The efficient catalytic degradation of naphthol was mainly attributed to the photolysis of iron oxalate complexes formed on iron mineral, which can accelerate the production of O₂^·-. Additionally, the produced Fe(Ⅱ) can accelerate the generation of ·OH via Fenton reaction. The findings can provide guidance for the development of green environmental water pollutant control technology using natural minerals.

Key words： iron mineral oxalate heterogeneous Fenton polycyclic aromatic hydrocarbon (PAHs) mechanism

收稿日期: 2023-03-23

PACS:

X52

基金资助:山东省地下水环境保护与修复工程技术研究中心开放基金资助项目（801KF2021-13）；国家自然科学基金资助项目（22176212）；江苏省“双创博士”基金资助项目（JSSCBS20211225）

通讯作者: 王坤,副教授,kwang@cumt.edu.cn E-mail: kwang@cumt.edu.cn

作者简介: 胡彩萍(1976-),女,山东西人,研究员,硕士,主要从事地质勘查、生态修复、地热勘查方向研究.发表论文20余篇.caipinghu126@126.com.

引用本文:

胡彩萍, 锁进然, 丁冠涛, 徐天缘, 魏善明, 王坤. 草酸强化天然铁矿石异相光助Fenton催化降解萘酚[J]. 中国环境科学, 2023, 43(11): 6016-6024. HU Cai-ping, SUO Jin-ran, DING Guan-tao, XU Tian-yuan, WEI Shan-ming, WANG Kun. Oxalate enhanced heterogeneous photo-Fenton activity of natural iron mineral for naphthol degradation. CHINA ENVIRONMENTAL SCIENCECE, 2023, 43(11): 6016-6024.

链接本文:

http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2023/V43/I11/6016

[1]	Kim K H, Jahan S A, Kabir E, et al. A review of airborne polycyclic aromatic hydrocarbons (PAHs) and their human health effects [J]. Environment International, 2013,60:71-80.
[2]	Haritash A, Kaushik C. Biodegradation aspects of polycyclic aromatic hydrocarbons (PAHs):a review [J]. Journal of Hazardous Materials, 2009,169:1-15.
[3]	Han J, Liang Y, Zhao B, et al. Polycyclic aromatic hydrocarbon (PAHs) geographical distribution in China and their source, risk assessment analysis [J]. Environmental Pollution, 2019,251:312-327.
[4]	刘明洋,李会茹,宋爱民,等.环境和人体中氯代/溴代多环芳烃的研究进展-污染来源、分析方法和污染特征[J]. 中国环境科学, 2021, 41(4):1842-1855. Liu M Y, Li H r, Song A m et al. A review of chlorinated/brominated polycyclic aromatic hydrocarbons in the environment and human:Sources, analysis methods and pollution characteristics. [J]. China Environmental Science, 2021,41(4):1842-1855.
[5]	Ghosal D, Ghosh S, Dutta T K, et al. Current state of knowledge in microbial degradation of polycyclic aromatic hydrocarbons (PAHs):A review [J]. Frontiers in Microbiology, 2016, 7:1369.
[6]	Suryanto B H, Wang Y, Hocking R K, et al. Overall electrochemical splitting of water at the heterogeneous interface of nickel and iron oxide [J]. Nature Communications, 2019,10:5599.
[7]	Mana S C A, Hanafiah M M, Chowdhury A J K. Environmental characteristics of clay and clay-based minerals [J]. Geology, Ecology, and Landscapes, 2017,(1):155-161.
[8]	Wei K, Liu X, Cao S, et al. Fe2O3@FeB composites facilitate heterogeneous Fenton process by efficient Fe (III)/Fe (II) cycle and in-situ H2O2 generation [J]. Chemical Engineering Journal Advances, 2021,8:100165.
[9]	Zhong Y, Liang X, He Z, et al. The constraints of transition metal substitutions (Ti, Cr, Mn, Co and Ni) in magnetite on its catalytic activity in heterogeneous Fenton and UV/Fenton reaction:From the perspective of hydroxyl radical generation [J]. Applied Catalysis B:Environmental, 2014,150:612-618.
[10]	He H, Zhong Y, Liang X, et al. Natural magnetite:An efficient catalyst for the degradation of organic contaminant [J]. Scientific Reports, 2015,5:1-10.
[11]	Munoz M, De Pedro Z M, Casas J A, et al. Preparation of magnetite-based catalysts and their application in heterogeneous Fenton oxidation-a review [J]. Applied Catalysis B:Environmental, 2015,176:249-265.
[12]	Sun H, Xie G, He D, et al. Ascorbic acid promoted magnetite Fenton degradation of alachlor:Mechanistic insights and kinetic modeling [J]. Applied Catalysis B:Environmental, 2020,267:118383.
[13]	Wang K, Wang C Y, Ren Z Y. Apatite-hosted melt inclusions from the Panzhihua gabbroic-layered intrusion associated with a giant Fe-Ti oxide deposit in SW China:insights for magma unmixing within a crystal mush [J]. Contributions to Mineralogy and Petrology, 2018, 173:1-14.
[14]	Wang k, Dong H, Ou Q, et al. Large-scale liquid immiscibility in the Hongge layered intrusion hosting a giant Fe-Ti oxide deposit in SW China [J]. Ore Geology Reviews, 2021,136:104268.
[15]	黄涛.安徽省马鞍山市象塘铁矿地质特征及成因[J]. 金属矿山, 2019,9:141-146. Huang Tao. Geological characteristics and genesis of Xiangtang Iron Deposit in Maanshan City, Anhui Province [J]. Metal Mine, 2019,9:141-146.
[16]	Zhang M H, Dong H, Zhao L, et al. A review on Fenton process for organic wastewater treatment based on optimization perspective [J]. Science of the Total Environment, 2019,670:110-121.
[17]	谢欣卓,钟金魁,李静,等.Fe3O4-nZVI类Fenton法降解水中磺胺甲恶唑谢[J]. 中国环境科学, 2022,42(7):3103-3111. Xie X Z, Zhong J K, Li J, et al. Degradation of sulfamethoxazole in water by Fenton-like method using Fe3O4-nZVI [J]. China Environmental Science, 2022,42(7):3103-3111.
[18]	Xu T, Zhu R, Zhu G, et al. Mechanisms for the enhanced photo-Fenton activity of ferrihydrite modified with BiVO4 at neutral pH [J]. Applied Catalysis B:Environmental, 2017,212:50-58.
[19]	Xu T, Zhu R, Shang H, et al. Photochemical behavior of ferrihydrite-oxalate system:Interfacial reaction mechanism and charge transfer process [J]. Water Research, 2019,159:10-19.
[20]	Li F, Koopal L, Tan W. Roles of different types of oxalate surface complexes in dissolution process of ferrihydrite aggregates [J]. Scientific Reports, 2018,8:1-13.
[21]	Tyutereva Y E, Sherin P S, Polyakova E V, et al. Photodegradation of para-arsanilic acid mediated by photolysis of iron (III) oxalate complexes [J]. Chemosphere, 2020,261:127770.
[22]	Pang H, Zhang Q, Wang H, et al. Photochemical aging of guaiacol by Fe (III)-oxalate complexes in atmospheric aqueous phase [J]. Environmental Science & Technology, 2018,53:127-136.
[23]	Salazar C, Nanny M A. Influence of hydrogen bonding upon the TiO2 photooxidation of isopropanol and acetone in aqueous solution [J]. Journal of Catalysis, 2010,269:404-410.
[24]	Yang Y Y, Zhang X G, Niu C G, et al. Dual-channel charges transfer strategy with synergistic effect of Z-scheme heterojunction and LSPR effect for enhanced quasi-full-spectrum photocatalytic bacterial inactivation:new insight into interfacial charge transfer and molecular oxygen activation [J]. Applied Catalysis B:Environmental, 2020,264:118465.
[25]	Jian H, Fang Y, Yue G, et al. Efficient removal of pyrene by biochar supported iron oxide in heterogeneous Fenton-like reaction via radicals and high-valent iron-oxo species [J]. Separation and Purification Technology, 2021,265:118518.
[26]	Radu T, Petran A, Olteanu D, et al. Evaluation of physico-chemical properties and biocompatibility of new surface functionalized Fe3O4 clusters of nanoparticles [J]. Applied Surface Science, 2020,501:144267.
[27]	Xu T, Fang Y, Tong T, et al. Environmental photochemistry in hematite-oxalate system:Fe(III)-Oxalate complex photolysis and ROS generation [J]. Applied Catalysis B:Environmental, 2021,283:119645.
[28]	Kuznetsov M, Zhuravlev J F, Gubanov V. XPS analysis of adsorption of oxygen molecules on the surface of Ti and TiNx films in vacuum [J]. Journal of Electron Spectroscopy and Related Phenomena, 1992,58:169-176.
[29]	Pang F, Zhang R, Lan D, et al. Synthesis of magnetite-semiconductor-metal trimer nanoparticles through functional modular assembly:a magnetically separable photocatalyst with photothermic enhancement for water reduction [J]. ACS Applied Materials & Interfaces, 2018,10:4929-4936.
[30]	Xue X, Hanna K, Despas C, et al. Effect of chelating agent on the oxidation rate of PCP in the magnetite/H2O2 system at neutral pH [J]. Journal of Molecular Catalysis A:Chemical, 2009,311:29-35.
[31]	Park J S, Wood P M, Davies M J, et al. A kinetic and ESR investigation of iron (II) oxalate oxidation by hydrogen peroxide and dioxygen as a source of hydroxyl radicals [J]. Free Radical Research, 1997,27:447-458.
[32]	Wang Z, Xiao D, Liu J. Diverse redox chemistry of photo/ferrioxalate system [J]. RSC Advances, 2014,4:44654.
[33]	Xu T, Zhu R, Shang H, et al. Photochemical behavior of ferrihydrite-oxalate system:Interfacial reaction mechanism and charge transfer process [J]. Water Research, 2019,159:10-19.