化工进展 ›› 2017, Vol. 36 ›› Issue (12): 4700-4707.DOI: 10.16085/j.issn.1000-6613.2017-0455

• 资源与环境化工 • 上一篇    

多孔材料Cu3(BTB)2和H2O2处理偶氮染料废水及机理

徐言慧1,2, 尹显洪1, 邱江源1, 黄在银1,2, 谭春萍3, 胡玉平1,2   

  1. 1 广西民族大学化学化工学院, 广西 南宁 530006;
    2 广西林产化学与工程重点实验室, 广西 南宁 530006;
    3 南宁学院, 广西 南宁 530200
  • 收稿日期:2017-03-20 修回日期:2017-05-26 出版日期:2017-12-05 发布日期:2017-12-05
  • 通讯作者: 胡玉平,博士,副教授,研究方向为环境化学与新材料。
  • 作者简介:徐言慧(1992-),女,硕士研究生。
  • 基金资助:
    国家自然科学基金(21267003)、广西高校科研项目(201203YB061)、广西民族大学2016年研究生科研创新计划(gxun-chxps201678)及广西民族大学引进人才科研启动项目(2013QD016)。

Application and mechanism of azo dye wastewater treatment using Cu3(BTB)2 and H2O2

XU Yanhui1,2, YIN Xianhong1, QIU Jiangyuan1, HUANG Zaiyin1,2, TAN Chunping3, HU Yuping1,2   

  1. 1 School of Chemistry and Chemical Engineering, Guangxi University for Nationalities, Nanning 530006, Guangxi, China;
    2 Guangxi Key Laboratory of Chemistry and Engineering of Forest Products, Nanning 530006, Guangxi, China;
    3 Nanning University, Nanning 530200, Guangxi, China
  • Received:2017-03-20 Revised:2017-05-26 Online:2017-12-05 Published:2017-12-05

摘要: 采用溶剂热法合成了Cu3(BTB)2(BTB=4,4',4"-benzenetri benzoate)介孔材料,并进行了SEM、BET、FTIR和XRD表征。该材料呈多孔球形,比表面积为1293m2/g,平均粒径为10μm。应用该材料进行刚果红偶氮染料废水处理,发现Cu3(BTB)2单独作用时,废水去除率为10.29%;Cu3(BTB)2和H2O2共同作用,去除率骤增到91.65%。通过紫外-可见光谱、高效液相色谱、微量热、捕获剂等手段分析其降解机理,Cu3(BTB)2与H2O2共存时,342nm处紫外特征吸收峰右移,HPLC峰强度显著降低,放热反应标准摩尔反应焓为2068.74kJ/mol,加入自由基捕获剂异丙醇或氯仿后,去除率大幅降低。实验结果表明:Cu3(BTB)2单独作用为多孔吸附,去除率较低,与H2O2共存时去除率高,归结于Fenton-like反应产生活性自由基(·OH和O2-)使CR分子键断裂,且·OH占主导作用。

关键词: 金属-有机框架化合物, Cu3(BTB)2, 过氧化氢, 吸附, 降解, 焓, 自由基

Abstract: The mesoporous materials Cu3(BTB)2(BTB=4,4',4"-benzenetri benzoate)was synthesized, and then characterized by scanning electron microscopy(SEM),nitrogen adsorption measurements(BET), Fourier transform infrared spectrometer(FTIR),and X-ray powder diffraction(XRD). The results show that the Cu3(BTB)2 particles were spherical,with a SBET of 1293m2/g, and an average particle size of 10μm. In the treatment of Congo red dye wastewater by using Cu3(BTB)2 alone, the removal rate was 10.29%, whereas treated by Cu3(BTB)2 and hydrogen peroxide(H2O2)together,the rate was increased to 91.65%. The mechanism was studied by means of UV-Vis spectroscopy,high performance liquid chromatography,microcalorimetry and free radical trapping agent. When Cu3(BTB)2 interacted with H2O2,the UV absorption peak at 342nm shifted to the right,the peak intensity of HPLC was reduced by about 500mV,and the exothermic standard molar reaction enthalpy was 2068.74kJ/mol. When we added opropanol(IPA)or chloroform(CF)to capture the ·OH or ·O2- radical into the reaction solution,the is removal rate was decreased. The results showed that Cu3(BTB)2 porous material could adsorb the CR dye,while H2O2 could produce the ·OH and ·O2- free-radical to break the CR molecular bond through the Fenton-like reaction,and the OH radicals played a dominant role.

Key words: metal-organic framework(MOF), Cu3(BTB)2, hydroen peroxide(H2O2)adsorption, degradation, enthalpy, radical

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