nav emailalert searchbtn searchbox tablepage yinyongbenwen piczone journalimg journalInfo journalinfonormal searchdiv searchzone qikanlogo popupnotification paper paperNew
2026, 03, v.47 119-126
铁氧化物吸附/共沉淀土壤有机质类芬顿降解对硝基苯酚
基金项目(Foundation): 国家自然科学基金项目(42577020、42207288)
邮箱(Email): ghy2721@sina.com;
DOI: 10.13291/j.cnki.djdxac.2026.03.014
发布时间: 2026-06-09
出版时间: 2026-06-09
网络发布时间: 2026-06-09
移动端阅读
摘要:

通过吸附和共沉淀两种方式制备具有不同C/Fe物质的量比(0~1.4)的铁氧化物-土壤有机质复合物(FhAx和FhCx),用于高效活化过氧化氢(H_2O2)降解对硝基苯酚(PNP)。研究表明,FhA和FhC均可促进PNP的类芬顿降解,且相同C/Fe比条件下,FhC相比于FhA具有更高催化活性。PNP的降解符合准一级动力学,FhC0.2具有更高的催化活性,其降解速率常数(0.013 7 min-1)分别是Fh/H_2O2、FhA0.2/H_2O2、FhA0.8/H_2O2、FhA1.4/H_2O2、FhC0.8/H_2O2和FhC1.4/H_2O2体系的2.1、1.4、3.0、2.7、1.4和1.2倍。FhC0.2/H_2O2体系PNP降解的最优pH为3,与pH为4、5和7的体系相比,其降解速率常数分别提高了27.4、45.6和68.5倍。4次循环实验后,FhC0.2降解率仍接近80%,反应前X射线衍射谱图发现材料未发生明显变化,说明其具有较高的结构稳定性。淬灭实验表明,FhC0.2活化H_2O2体系中产生的主要活性氧物种是羟基自由基(·OH)。研究结果有望揭示Fe-C复合材料的作用形式在类芬顿降解有机污染物过程的影响,并为其主要催化机制提供新的见解。

Abstract:

In this study, iron oxide-soil organic complexes prepared via adsorption(FhAx, x represents C/Fe molar ratio) and coprecipitation(FhCx) with different C/Fe molar ratios(0-1.4) were synthesized and used as catalysts for H_2O2 activation and p-nitrophenol(PNP) degradation. Both FhA and FhC could promote the Fenton-like degradation of PNP, and FhC exhibited higher catalytic activity than FhA under the same C/Fe molar ratios. The degradation of PNP followed pseudo-first-order kinetics. The rate constant of PNP degradation of FhC0.2/H_2O2 system(0.013 7 min-1) was 2.1, 1.4, 3.0, 2.7, 1.4 and 1.2 folds higher of Fh/H_2O2, FhA0.2/H_2O2, FhA0.8/H_2O2, FhA1.4/H_2O2, FhC0.8/H_2O2 and FhC1.4/H_2O2, respectively. The optimal pH for PNP degradation in the FhC0.2/H_2O2 system was 3, and the degradation rate constant of PNP degradation at pH 3 was 27.4, 45.6, and 68.5 times higher than those at pH 4, 5, and 7, respectively. After 4 cycles, FhC0.2 maintained nearly 80% degradation efficiency, and XRD patterns showed no significant change, indicating high structural stability.Quenching experiment demonstrated that hydroxyl radical(~.OH) was the main reactive oxygen species during the Fenton-like degradation of PNP mediated by FhC0.2. This study revealed the effects of the forms(adsorption vs. coprecipitation) of Fe-C complexes on the Fenton-like degradation of organic pollutants and provided new insights into the main catalytic mechanisms mediated by Fe-C complexes.

参考文献

[1]WEI J,SONG Y,TU X,et al.Pretreatment of dry-spun acrylic fiber manufacturing wastewater by Fenton process:optimization,kinetics and mechanisms [J].Chemical Engineering Journal,2013,218:218319-218326.

[2]ZHU Y P,ZHU R L,XI Y F,et al.Strategies for enhancing the heterogeneous Fenton catalytic reactivity:a review [J].Applied Catalysis B:Environmental,2019,255:117739.

[3]PHAM A L,DOYLE F M,SEDLAK D L.Kinetics and efficiency of H2O2 activation by iron-containing minerals and aquifer materials [J].Water Research,2012,46:6454-6462.

[4]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,2009,11:29-35.

[5]SONG W,CHENGM,MA J,et al.Decomposition of hydrogen peroxide driven by photochemical cycling of iron species in clay [J].Environmental Science & Technology,2006,40:4782-4787.

[6]ANNETTE P,CHRISTAIN S,ANDREAS K.Electron transfer from humic substances to biogenic and abiogenic Fe(III) oxyhydroxide minerals [J].Environmental Science & Technology,2014,48:1656-1664.

[7]ROMERO A,SANTOS A,VICENTE F,et al.In situ oxidation remediation technologies:kinetic of hydrogen peroxide decomposition on soil organic matter [J].Journal of Hazardous Materials,2009,170:627-632.

[8]LIN Z,ZHAO L,DONG Y.Effects of low molecular weight organic acids and fulvic acid on 2,4,4′-trichlorobiphenyl degradation and hydroxyl radical formation in a goethite-catalyzed Fenton-like reaction [J].Chemical Engineering Journal,2017,326:201-209.

[9]XU J,FAN X,HUANG F,et al.Iron bound to soil organic matter catalyzes H2O2 to oxidize crude oil in soil [J].Journal of Hazardous Materials,2017,322:516-524.

[10]FARINELLI G,MINELLA M,PAZZI M,et al.Natural iron ligands promote a metal-based oxidation mechanism for the Fenton reaction in water environments [J].Journal of Hazardous Materials,2020,393:122413.

[11]YU H,LIU G,SHEN L,et al.Goethite-humic acid coprecipitate mediated Fenton-like degradation of sulfanilamide:the role of coprecipitated humic acid in accelerating Fe(III)/Fe(II) cycle and degradation efficiency [J].Journal of Hazardous Materials,2020,403:124026.

[12]CHEN C,DYNES J J,WANG J,et al.Properties of Fe-organic matter associations via coprecipitation versus adsorption [J].Environmental Science & Technology,2014,48:13751-13759.

[13]YANG R,TAO J,HUANG Q,et al.Co-adsorption of Cd(II) and Sb(III) by ferrihydrite:a combined XPS and ITC study [J].Journal of Soils and Sediments,2019,19:1319-1327.

[14]WEI J,ZHANG F,HE T,et al.Selective associations of organic matter components with ferrihydrite:implications for Fe-organic matter preservation in tidal flat wetlands [J].Geoderma,2023,437:116574.

[15]XU M,ZHAO Z,SHI M,et al.Effect of humic acid on the stabilization of cadmium in soil by coprecipitating with ferrihydrite [J].Environmental Science and Pollution Research International,2019,26:27330-27337.

[16]MIKUTTA R,LORENZ D,GUGGENBERGER G,et al.Properties and reactivity of Fe-organic matter associations formed by coprecipitation versus adsorption:clues from arsenate batch adsorption [J].Geochimica et Cosmochimica Acta,2014,144:258-276.

[17]YU H,LIU G,SHEN L,et al.Facile preparation of coprecipitates between iron oxides and dissolved organic matter for efficient Fenton-like degradation of norfloxacin [J].Journal of Hazardous Materials,2023,444:130394-130394.

[18]FENG J,HU X,YUE P.Effect of initial solution pH on the degradation of OrangeⅡ using clay-based Fe nanocomposites as heterogeneous photo-Fenton catalyst [J].Water Research,2005,40:641-646.

[19]YE Q,WU J,WU P,et al.Enhancing peroxymonosulfate activation of Fe-Al layered double hydroxide by dissolved organic matter:performance and mechanism [J].Water Research,2020,185:116246.

[20]LEE H,KIM H I,WEON S,et al.Activation of persulfates by graphitized nanodiamonds for removal of organic compounds [J].Environmental Sscience & Technology,2016,50:10134-10142.

[21]PIEPENBROCK A,SCHRODER C,KAPPLER A.Electron transfer from humic substances to biogenic and abiogenic Fe(Ⅲ) oxyhydroxide minerals [J].Environmental Science & Technology,2014,48:1656-1664.

[22]ROYER R A,BURGOS W D,FISHER A S,et al.Enhancement of biological reduction of hematite by electron shuttling and Fe(Ⅱ) complexation [J].Environmental Science & Technology,2002,36:1939-1946.

基本信息:

DOI:10.13291/j.cnki.djdxac.2026.03.014

中图分类号:TQ426;O647.3;X53

引用信息:

[1]于华莉,郭子康,梁金辉,等.铁氧化物吸附/共沉淀土壤有机质类芬顿降解对硝基苯酚[J].大连交通大学学报,2026,47(03):119-126.DOI:10.13291/j.cnki.djdxac.2026.03.014.

基金信息:

国家自然科学基金项目(42577020、42207288)

发布时间:

2026-06-09

出版时间:

2026-06-09

网络发布时间:

2026-06-09

检 索 高级检索

引用

GB/T 7714-2015 格式引文
MLA格式引文
APA格式引文