物理化学学报
物理化學學報
물이화학학보
ACTA PHYSICO-CHIMICA SINICA
2015年
4期
771-782
,共12页
胡龙兴%许丹丹%邹联沛%袁航%胡星
鬍龍興%許丹丹%鄒聯沛%袁航%鬍星
호룡흥%허단단%추련패%원항%호성
非均相芬顿氧化%吸附%Fe/SBA-15%罗丹明B%羟基自由基
非均相芬頓氧化%吸附%Fe/SBA-15%囉丹明B%羥基自由基
비균상분돈양화%흡부%Fe/SBA-15%라단명B%간기자유기
Heterogeneous Fenton oxidation%Adsorption%Fe/SBA-15%Rhodamine B%Hydroxyl radical
以介孔二氧化硅SBA-15为载体,采用等体积浸渍法制备了Fe/SBA-15.通过X射线衍射(XRD)、N2吸附-脱附、扫描电镜(SEM)、透射电镜(TEM)和X射线光电子能谱(XPS)等技术对其进行了表征,并用于对水溶液中罗丹明B (RhB)的芬顿氧化.表征结果表明了Fe/SBA-15维持了长程有序的介孔结构,孔径和比表面积都有所下降,并呈现棒状体的聚集态,平均直径为0.6μm. Fe以α-Fe2O3的形态同时存在于介孔孔道内外.在Fe/SBA-15和H2O2同时存在条件下RhB的去除是吸附和催化氧化降解的协同作用所致,并且与Fe/SBA-15投加量密切相关,但与初始溶液pH几乎无关.当Fe/SBA-15投加量为0.15 g?L-1, RhB初始浓度为10.0 mg?L-1, H2O2/Fe3+摩尔比为2000:1,初始溶液pH为5.4和反应温度为21°C时, RhB去除率达到了93%. Fe/SBA-15的Langmiur单分子层饱和吸附量为99.11 mg?g-1.此外,采用H2O2浸泡方式对使用过的Fe/SBA-15可进行再生,连续6次循环使用后仍可维持80%的RhB去除率,且每次使用后Fe浸出浓度都在0.1 mg?L-1(或者0.6%(质量分数))以下.基于淬灭实验、UV-Vis光谱和气相色谱-质谱(GC-MS)联用仪分析的结果,提出了RhB的去除机理.非均相芬顿催化剂Fe/SBA-15可用于去除像RhB这样的生物难降解有机物.
以介孔二氧化硅SBA-15為載體,採用等體積浸漬法製備瞭Fe/SBA-15.通過X射線衍射(XRD)、N2吸附-脫附、掃描電鏡(SEM)、透射電鏡(TEM)和X射線光電子能譜(XPS)等技術對其進行瞭錶徵,併用于對水溶液中囉丹明B (RhB)的芬頓氧化.錶徵結果錶明瞭Fe/SBA-15維持瞭長程有序的介孔結構,孔徑和比錶麵積都有所下降,併呈現棒狀體的聚集態,平均直徑為0.6μm. Fe以α-Fe2O3的形態同時存在于介孔孔道內外.在Fe/SBA-15和H2O2同時存在條件下RhB的去除是吸附和催化氧化降解的協同作用所緻,併且與Fe/SBA-15投加量密切相關,但與初始溶液pH幾乎無關.噹Fe/SBA-15投加量為0.15 g?L-1, RhB初始濃度為10.0 mg?L-1, H2O2/Fe3+摩爾比為2000:1,初始溶液pH為5.4和反應溫度為21°C時, RhB去除率達到瞭93%. Fe/SBA-15的Langmiur單分子層飽和吸附量為99.11 mg?g-1.此外,採用H2O2浸泡方式對使用過的Fe/SBA-15可進行再生,連續6次循環使用後仍可維持80%的RhB去除率,且每次使用後Fe浸齣濃度都在0.1 mg?L-1(或者0.6%(質量分數))以下.基于淬滅實驗、UV-Vis光譜和氣相色譜-質譜(GC-MS)聯用儀分析的結果,提齣瞭RhB的去除機理.非均相芬頓催化劑Fe/SBA-15可用于去除像RhB這樣的生物難降解有機物.
이개공이양화규SBA-15위재체,채용등체적침지법제비료Fe/SBA-15.통과X사선연사(XRD)、N2흡부-탈부、소묘전경(SEM)、투사전경(TEM)화X사선광전자능보(XPS)등기술대기진행료표정,병용우대수용액중라단명B (RhB)적분돈양화.표정결과표명료Fe/SBA-15유지료장정유서적개공결구,공경화비표면적도유소하강,병정현봉상체적취집태,평균직경위0.6μm. Fe이α-Fe2O3적형태동시존재우개공공도내외.재Fe/SBA-15화H2O2동시존재조건하RhB적거제시흡부화최화양화강해적협동작용소치,병차여Fe/SBA-15투가량밀절상관,단여초시용액pH궤호무관.당Fe/SBA-15투가량위0.15 g?L-1, RhB초시농도위10.0 mg?L-1, H2O2/Fe3+마이비위2000:1,초시용액pH위5.4화반응온도위21°C시, RhB거제솔체도료93%. Fe/SBA-15적Langmiur단분자층포화흡부량위99.11 mg?g-1.차외,채용H2O2침포방식대사용과적Fe/SBA-15가진행재생,련속6차순배사용후잉가유지80%적RhB거제솔,차매차사용후Fe침출농도도재0.1 mg?L-1(혹자0.6%(질량분수))이하.기우쉬멸실험、UV-Vis광보화기상색보-질보(GC-MS)련용의분석적결과,제출료RhB적거제궤리.비균상분돈최화제Fe/SBA-15가용우거제상RhB저양적생물난강해유궤물.
An Fe-loaded mesoporous silica SBA-15, Fe/SBA-15, was prepared by incipient wetness impregnation, characterized by X-ray diffraction (XRD), N2 adsorption-desorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) techniques and used for heterogeneous Fenton oxidation of dye Rhodamine B (RhB) in aqueous solution. The characterization showed that the Fe/SBA-15 retained a mesoporous structure with a long-range ordered arrangement, reduced pore diameter and surface area, and existed as agglomerates of rod-like crystal ites with a mean diameter of 0.6μm. The Fe species occurred both inside and outside the support pores in the form ofα-Fe2O3 crystal ites. The removal of RhB in the presence of Fe/SBA-15 and H2O2 was shown to be caused by the synergistic effects of adsorption and catalytic oxidative degradation, and was closely related to Fe/SBA-15 dosage. Removal was almost independent of initial solution pH, with approximately 93%achieved at an Fe/SBA-15 dosage of 0.15 g?L-1, initial RhB concentration of 10.0 mg?L-1, H2O2/Fe3+molar ratio of 2000:1;initial solution pH of 5.4 and 21 °C. The Langmuir monolayer adsorption capacity of the Fe/SBA-15 was 99.11 mg?g-1. In addition, Fe/SBA-15 can be easily regenerated by soaking in H2O2 then reused for up to six runs, with RhB removal greater than 80%and Fe leaching below 0.1 mg?L-1 (or 0.6%(mass fraction)) for each run. A removal mechanism for RhB by Fe/
<br> SBA-15 and H2O2 was proposed based on the quenching tests, UV-Vis spectra, and gas chromatography-mass spectrometry (GC-MS) analysis. The heterogeneous Fenton catalyst Fe/SBA-15 can be applied to remove non-biodegradable organics such as dye RhB.