13 | 0 | 9 |
下载次数 | 被引频次 | 阅读次数 |
[目的]研究FeS2催化降解苯酚的效果。[方法]采用简易的水热法,以Fe(NO3)2·6H2O和Na2S为原料成功制备了纳米片状FeS2材料,采用X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电镜(TEM)、X射线光电子能谱(XPS)、N2等温吸附/脱附等手段,对FeS2样品的组成和微观结构进行表征。以降解水体有机污染物苯酚为目标,研究了FeS2对过硫酸钠(PS)的活化效果,考察了反应条件对苯酚降解率的影响。[结果]所制FeS2具有介孔结构,比表面积高达136.7 m2/g,其中的Fe主要是以Fe2+的形式存在。它能够有效活化PS降解苯酚,降解反应的最佳条件为:FeS2质量浓度2.2 g/L,PS与苯酚的物质的量比40∶1,苯酚初始质量浓度25 mg/L,体系的pH=3.8,反应温度30°C,反应时间7.5 h。在最佳的反应条件下,苯酚的降解率高达99.5%。自由基淬灭实验结果表明,·SO4-是降解苯酚的主导氧化剂。[结论]纳米片状FeS2对苯酚的降解有良好的催化活性。
Abstract:[Objective]It is worthy to study the catalytic performance of iron disulfide (FeS2) in phenol degradation.[Method]FeS2 nanosheets were synthesized via a facile hydrothermal method using and Fe(NO3)2·6H2O and Na2S.The composition and microstructure of FeS2 were characterized by X-ray diffraction (XRD),scanning electron microscopy(SEM),transmission electron microscopy (TEM),X-ray photoelectron spectroscopy (XPS),and N2 adsorption/desorption isotherm measurement.Aiming at the degradation of phenol (a common organic contaminant) in water,the activation of sodium persulfate (PS) by FeS2 and the effects of various reaction conditions on phenol degradation efficiency were studied.[Result]FeS2 had a mesoporous structure with a specific surface area as high as 136.7 m2/g,contained predominantly Fe2+species,and effectively activated PS to degrade phenol.The phenol degradation efficiency reached up to 99.5%under the following optimized degradation conditions:FeS2 2.2 g/L,PS-to-phenol molar ratio 40:1,initial phenol concentration 25 mg/L,pH 3.8,reaction temperature 30℃,and reaction time 7.5 h.The result of free radical quenching experiment confirmed sulfate radicals as the primary oxidizing species.[Conclusion]Fe S2 nanosheets exhibits excellent catalytic activity for phenol degradation via persulfate activation.
[1]高焕方,龙飞,曹园城,等.新型过硫酸盐活化技术降解有机污染物的研究进展[J].环境工程学报, 2015, 9(12):5659-5664.GAO H F, LONG F, CAO Y C, et al. Advances in degradation of organic pollutants by novel persulfate activated technology[J].Chinese Journal of Environmental Engineering, 2015, 9(12):5659-5664.
[2]黄智辉,纪志永,陈希,等.过硫酸盐高级氧化降解水体中有机污染物研究进展[J].化工进展, 2019, 38(5):2461-2470.HUANG Z H, JI Z Y, CHEN X, et al. Degradation of organic pollutants in water by persulfate advanced oxidation[J]. Chemical Industry and Engineering Progress, 2019, 38(5):2461-2470.
[3]樊茹沛,张国珍,周添红,等.过硫酸盐氧化法降解水中有机物的研究进展[J].应用化工, 2021, 50(2):470-475.FAN R P, ZHANG G Z, ZHOU T H, et al. Research progress on the treatment of organic matter in wastewater by persulfate oxidation technology[J]. Applied Chemical Industry, 2021, 50(2):470-475.
[4]孙二军,常玉,姜露雨,等.长链锌卟啉/氧化石墨烯复合材料的制备及其光降解亚甲基蓝研究[J].化工新型材料, 2021, 49(9):276-279.SUN E J, CHANG Y, JIANG L Y, et al. Preparation of Zn–P/GO composite and its photo-degradation of methylene blue[J]. New Chemical Materials, 2021, 49(9):276-279.
[5]王琦瑞,史怡璇,吕诗怡,等.炭材料负载金属催化剂在活化过硫酸盐中的应用进展[J].化工新型材料, 2021, 49(2):64-67.WANG Q R, SHI Y X, LYU S Y, et al. Application progress of carbon material supported metal catalyst in activation of persulfate[J].New Chemical Materials, 2021, 49(9):276-279.
[6]MA J, LI H Y, CHI L P, et al. Changes in activation energy and kinetics of heat-activated persulfate oxidation of phenol in response to changes in pH and temperature[J]. Chemosphere, 2017, 189:86-93.
[7]张昊楠,唐海,沙俊鹏,等.热辅助CuO/ZSM-5活化过硫酸盐降解苯酚废水研究[J].化工新型材料, 2017, 45(3):186-189.ZHANG H N, TANG H, SHA J P, et al. Research on degradation of phenol wastewater sued CuO/ZSM-5 activated persulfate assisted by thermo process[J]. New Chemical Materials, 2017, 45(3):186-189.
[8]邵强,郭轶琼.铁锰催化剂活化过硫酸盐去除水中苯酚的研究[J].工业水处理, 2020, 40(7):94-97.SHAO Q, GUO T Q. Removal of phenol from water by activation of persulfate with Fe–Mn catalyst[J]. Industrial Water Treatment, 2020,40(7):94-97.
[9]BAE S J, KIM D W, LEE W J. Degradation of diclofenac by pyrite catalyzed Fenton oxidation[J]. Applied Catalysis B:Environmental,2013, 134/135:93-102.
[10]白静,扶咏梅,王文琪,等.非均相催化过硫酸盐氧化技术研究进展[J].化工环保, 2019, 39(3):247-254.BAI J, FU Y M, WANG W Q, et al. Research progresses on heterogeneous catalytic persulfate oxidation technology[J].Environmental Protection of Chemical Industry, 2019, 39(3):247-254.
[11]王一凡,李小蝶,侯美茹,等.锰基氧化物活化过硫酸盐降解水中有机污染物的研究进展[J].环境科学研究, 2021, 34(8):1899-1908.WANG Y F, LI X D, HOU M R, et al. Activation of persulfate with Mn-based oxides for degradation of organic pollutants in water:a review[J]. Research of Environmental Sciences, 2021, 34(8):1899-1908.
[12]钟仁华,黄启玉,吴大旺,等.纳米片状FeCo2O4材料的制备及其用于活化过硫酸盐催化降解苯酚的研究[J].电镀与涂饰, 2022, 41(8):578-584.ZHONG R H, HUANG Q Y, WU D W, et al. Study on preparation of FeCo04 nanosheet and its application in activation of persulfate for catalytic degradation of phenol[J]. Electroplating&Finishing, 2022,41(8):578-584.
[13]田婷婷,李朝阳,王召东,等.过渡金属活化过硫酸盐降解有机废水技术研究进展[J].化工进展, 2021, 40(6):3480-3488.TIAN T T, LI C Y, WANG S D, et al. Research progress of transition metal activated persulfate to degrade organic wastewater[J].Chemical Industry and Engineering Progress, 2021, 40(6):3480-3488.
[14]LI Y, BAGHI R, FILIP J, et al. Activation of peroxydisulfate by ferrite materials for phenol degradation[J]. ACS Sustainable Chemistry&Engineering, 2019, 7(9):8099-8108.
[15]LU Y S, WANG Z, XU Y F, et al. Fe2(MoO4)3 as a novel heterogeneous catalyst to activate persulfate for Rhodamine B degradation[J]. Desalination and Water Treatment, 2016, 57:7898-7909.
[16]ZHOU R,ZHAO J, SHEN N F, et al. Efficient degradation of2,4-dichlorophenol in aqueous solution by peroxymonosulfate activated with magnetic spinel FeCo2O4 nanoparticles[J].Chemosphere, 2018, 197:670-679.
[17]姚淑华,陈雪静,王海博.棒状FeMoO4材料的制备及其活化性能[J].精细化工, 2020, 37(5):1032-1037.YAO S H, CHEN X J, WANG H B. Preparation and activation properties of rod-shaped FeMoO, materials[J]. Fine Chemicals, 2020,37(5):1032-1037.
[18]DIAO Z H, XU X R, JIANG D, et al. Enhanced catalytic degradation of ciprofloxacin with FeS2/SiO2 microspheres as heterogeneous Fenton catalyst:Kinetics, reaction pathways and mechanism[J].Chemical Engineering Journal, 2017, 327:108-115.
[19]OH S Y, KANG S G, KIM D W, et al. Degradation of2,4-dinitrotoluene by persulfate activated with iron sulfides[J].Chemical Engineering Journal, 2011, 172(2/3):641-646.
[20]ASEMAN-BASHIZ E, SAYYAF H. Synthesis of nano-FeS2 and its application as an effective activator of ozone and peroxydisulfate in the electrochemical process for ofloxacin degradation:a comparative study[J]. Chemosphere, 2021, 274:129772.
[21]YAN S C, WANG K, ZHOU F, et al. Ultrafine Co:FeS2/CoS2heterostructure nanowires for highly efficient hydrogen evolution reaction[J]. ACS Applied Energy Materials, 2020, 3(1):514-520.
[22]BAI R L, LUO X H, ZHEN D S, et al. Facile fabrication of comb-like porous NiCo2O4 nanoneedles on Ni foam as an advanced electrode for high-performance supercapacitor[J]. International Journal of Hydrogen Energy, 2020, 45(56):32343-323543.
[23]ZHAO X, MA X, LU Q Q, et al. FeS2-doped MoS2 nanoflower with the dominant 1T-MoS2 phase as an excellent electrocatalyst for highperformance hydrogen evolution[J]. Electrochimica Acta, 2020, 249:72-78.
[24]YE Z H, PADILLA J A, XURIGUERA E, et al. A highly stable metal–organic framework-engineered FeS2/C nanocatalyst for heterogeneous electro-Fenton treatment:Validation in wastewater at mild pH[J]. Environmental Science&Technology, 2020, 54(7):4664-4674.
[25]CHEN Y, YAN J C, OUYANG D, et al. Heterogeneously catalyzed persulfate by CuMgFe layered double oxide for the degradation of phenol[J]. Applied Catalysis A:General, 2017, 538:19-26.
[26]MASOMBOON N, RATANATAMSKUL C, LU M C. Chemical oxidation of 2,6-dimethylaniline in the Fenton process[J].Environmental Science&Technology, 2009, 43(22):8629-8634.
[27]RAO Y F, QU L, YANG H, et al. Degradation of carbamazepine by Fe(II)-activated persulfate process[J]. Journal of Hazardous Materials,2014, 268:23-32.
[28]ZHANG Y Q, TRAN H P, DU X D, et al. Efficient pyrite activating persulfate process for degradation of p-chloroaniline in aqueous systems:a mechanistic study[J]. Chemical Engineering Journal, 2017,108:1112-1119.
[29]冯俊生,张郓,王晓红,等.石墨烯电极电活化过硫酸盐降解含酚废水研究[J].安全与环境学报, 2021, 21(1):404-410.FENG J S, ZHANG Y, WANG X H, et al. Degrading phenolic sewage via the graphene electrodes through the electrically activated persulfate[J]. Journal of Safety and Environment, 2021, 21(1):404-410.
基本信息:
DOI:10.19289/j.1004-227x.2025.05.022
中图分类号:X703;TQ426;TB383.1
引用信息:
[1]罗小虎,戴红,吴大旺等.纳米片状FeS_2的制备及催化降解苯酚性能的研究[J].电镀与涂饰,2025,44(05):139-145.DOI:10.19289/j.1004-227x.2025.05.022.
基金信息:
贵州省材料失效与防护工程研究中心(黔教技[2022]057号); 贵州省高等学校无机配位材料制造与新型功能化应用创新团队(黔教技[2023]090号); 贵州省教育厅自然科学研究项目(青年科技人才成长项目)(黔教技[2024]239号)