Cu/Fe掺杂Silicalite-1合成及其Fenton氧化含酚废水的试验研究  

Hydrothermal Synthesis of Silicalite-1 with Cu/Fe Doped and Used in Fenton Oxidation of Phenol Wastewater

作　　者：张新华[1,2,3] 包乐乐 王慧娟 杨期勇[2,3] 杨平华 

机构地区：[1]九江学院化学与环境工程学院,江西九江332005 [2]九江市流域管理与生态保护重点实验室,江西九江332005 [3]江西省生态化工工程技术中心,九江学院,江西九江332005

出　　处：《环境科学与技术》2017年第9期143-147,共5页Environmental Science & Technology

基　　金：国家自然科学基金(21567011);江西省自然科学基金项目(20151BA203043)

摘　　要：采用水热法合成了Cu,Fe掺杂的Silicalite-1分子筛,并用X衍射光谱(XRD),扫描电镜(SEM),X射线能谱(EDS),傅里叶红外光谱(FT-IR),N_2吸附/脱附以及原子吸收光谱(AAS)进行了表征。结果表明,合成的Cu,Fe掺杂Silicalite-1分子筛晶型完整,呈六方柱形,颗粒大小在1.5~3.5μm之间,Cu,Fe在Silicalite-1上呈高度分散状态。模拟苯酚废水的Fenton氧化实验表明,Cu,Fe能显著提高Silicalite-1对苯酚废水的催化反应活性,其中,2%-(Cu,Fe)-S-1效果最优。在p H为6.8,H_2O_2/Cat.=50∶1及环境温度条件下,经过3.0 h的反应后,2%-(Cu,Fe)-S-1对苯酚和COD的去除率分别可达93.2%和72.5%。当反应温度升高到308 K时,在相同的条件下,2%-(Cu,Fe)-S-1对苯酚和COD的去除率分别可达100%和94%,且Cu,Fe的溶出率较低。此外,Cu,Fe共掺杂的Silicalite-1比单掺杂时具有更好的反应活性,表明Cu和Fe对苯酚废水的降解具有协同作用。Four types of Silicalite-1 with Cu and Fe doped were synthesized by hydrothermal method and used in Fenton oxidation of phenol wastewater.Their physicochemical properties were characterized in detail by X-ray diffraction（XRD）,scanning electron microscope（SEM）, energy dispersive spectrometer（EDS）, Fourier transform infrared spectroscopy（FT-IR）,N2 adsorption/desorption and atomic absorption spectroscopy（AAS）. The results indicated that Cu and Fe doped Silicalite-1 were exhibited integrity hexagonal prism shapes with particle sizes distribution between 1.5 ~3.5 μm, and Cu and Fe were highly dispersed on the surface of Silicalite-1. The performance of Silicalite-1 in phenol wastewater degradation was signifi-cantly improved with Cu and Fe doped.2%-（Cu, Fe）-S-1 showed the best activity among all investigated samples. Under the conditions of p H 6.8, dosage of H2 O2/Cat.50∶1, the phenol and COD removal efficiencies of 2%-（Cu, Fe）-S-1 reached 93.2%and 72.5%, respectively, after 3.0 h of reaction at ambient temperature. As the reaction temperature increased to 308 K, the phenol and COD removal efficiencies of 2%-（Cu, Fe）-S-1 reached 100% and 94%, respectively, under the same conditions.The catalyst also showed comparable stability with low leaching out of Cu and Fe. Meanwhile, the higher phenol degradation activity of Silicalite-1 with Cu and Fe co-doped than that of Silicalite-1 with Cu or Fe mono-doped meant that Cu and Fe had synergistic effect in phenol wastewater degradation.

关 键 词：水热法 SILICALITE-1 Cu/Fe掺杂 FENTON氧化 含酚废水 

分 类 号：X506[环境科学与工程—环境工程]