催化学报

催化学报 ›› 2017, Vol. 38 ›› Issue (10): 1719-1725.DOI: 10.1016/S1872-2067(17)62884-5

• 论文 • 上一篇    下一篇

常温常压湿式催化氧化染料废水的Mo-Cu-Fe-O新型复合催化材料

许银, 邵贺楠, 葛飞, 刘云   

  1. 湘潭大学环境与资源学院环境科学与工程系, 湖南湘潭 411105
  • 收稿日期:2017-05-08 修回日期:2017-06-28 出版日期:2017-10-18 发布日期:2017-10-28
  • 通讯作者: 许银
  • 基金资助:

    国家自然科学基金（51678511，51308484）；湖南省自然科学基金（13JJ4049）；湖南省教育厅（14C1094）；中国科学院矿物学和成矿学重点实验室开放基金（KLMM20150104）；湘潭大学重大人才计划培育基金（16PYZ09）；湘潭大学博士启动项目（12QDZ18）。

Novel-structured Mo-Cu-Fe-O composite for catalytic air oxidation of dye-containing wastewater under ambient temperature and pressure

Yin Xu, Henan Shao, Fei Ge, Yun Liu   

  1. Department of Environmental Science and Engineering, College of Environment and Resources, Xiangtan University, Xiangtan 411105, Hunan, China
  • Received:2017-05-08 Revised:2017-06-28 Online:2017-10-18 Published:2017-10-28
  • Contact: 10.1016/S1872-2067(17)62884-5
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (51678511, 51308484), the Natural Science Foundation of Hunan Province (13JJ4049), the Education Department Fund of Hunan Province (14C1094), the Open Fund of Key Laboratory of Mineralogy and Metallogeny in Chinese Academy of Sciences (KLMM20150104), the Major Talent Training Program of Xiangtan University (16PYZ09), and the Specialized Research Fund for the Doctoral Program of Xiangtan University (12QDZ18).

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摘要：

染料广泛应用于纺织厂、皮革厂以及染发等各个领域.染料废水具有成分复杂、浓度高、色度大和生物难降解等特性，因此传统的处理方法难以将其完全降解.高级氧化技术已成为国内外广泛应用的染料废水处理技术之一，特别是湿式催化氧化（CWAO）技术.然而，CWAO工艺中反应往往需要高温（通常为200-280℃）和高压（通常为2-9 MPa），制约了其广泛应用.因此，人们致力于研发具有高催化活性的催化剂，通过改变反应历程和降低反应的活化能，使反应在常温常压条件下进行.
本课题组曾采用钼酸盐浸渍于Zn/Al LDHs溶液中成功制备了Mo/Zn-Al LDHs催化剂，该催化剂能在常温常压下湿式催化氧化降解阳离子红GTL有机废水.Mo/Zn-Al LDHs催化剂中Mo作为主催化成分，Zn-Al LDHs作为载体.Cu-Fe LDHs本身作为一种催化剂，与Mo相结合能有效提高催化剂的活性及稳定性，因此本文采用浸渍法制备了Mo-Cu-Fe-O新型复合催化材料，采用X射线衍射、氢气程序升温还原、循环伏安法和氧气程序升温脱附等表征手段研究了Mo-Cu-Fe-O材料的结构及氧化还原特性.以阳离子红GTL、结晶紫和酸性红为染料废水代表，研究了常温常压下Mo-Cu-Fe-O催化降解染料废水的催化活性.结果表明，在中性条件下Mo-Cu-Fe-O对阳离子型染料废水具有良好的催化活性.循环使用七次后该样品对阳离子红GTL和酸性红的脱色率分别达到91.5%和92.8%，然而对酸性红阴离子型染料废水基本无催化活性.在常温常压CWAO过程中产生的羟基自由基能有效降解阳离子GTL废水，其废水毒性随着反应的进行逐渐减小.

关键词: Mo-Cu-Fe-O催化剂, 常温常压, 染料废水, 羟基自由基, 氧化降解

Abstract:

A novel-structured Mo-Cu-Fe-O composite was successfully prepared by co-precipitation and impregnation method. The properties of the as-prepared samples were determined using X-ray diffraction, temperature-programmed reduction by H2, cyclic voltammetry, and temperature-programmed desorption by O2. The results showed that Mo6+ diffused into the Cu-Fe-O crystal lattice and then formed a new crystalline phase of CuMoO4. The Mo-Cu-Fe-O catalyst had redox properties, and its surface contained active sites for oxygen adsorption. In addition, the catalytic activity of the Mo-Cu-Fe-O composite was evaluated by the degradation of Cationic Red GTL, Crystal Violet, and Acid Red in catalytic wet air oxidation (CWAO) at ambient temperature and pressure. The Mo-Cu-Fe-O catalyst showed excellent activity at basic conditions for the degradation of Cationic Red GTL. High removal efficiencies of 91.5% and 92.8% were achieved for Cationic Red GTL and Crystal Violet, respectively, in wastewater, and the efficiency remained high after seven cycles. However, almost no degradation of Acid Red occurred in the CWAO process. Furthermore, hydroxyl radicals were formed in the CWAO process, which induced the decomposition of the two cationic dyes in wastewater, and the toxicity of their effluents was decreased after degradation. The results indicate that the Mo-Cu-Fe-O composite shows excellent catalytic activity for the treatment of wastewater contaminated with cationic dyes.

Key words: Mo-Cu-Fe-O catalyst, Ambient temperature and pressure, Dye wastewater, Hydroxyl radical, Oxidative degradation