研究报告

  • 姜理英,张瑜芬,胡俊,姚志伟,黄武,汤露.NTP协同双金属锰基催化剂降解氯苯的性能研究[J].环境科学学报,2021,41(3):922-931

  • NTP协同双金属锰基催化剂降解氯苯的性能研究
  • Removal of chlorobenzene by non-thermal plasma combined with bimetallic manganese-based catalyst
  • 基金项目:浙江省科技计划项目-公益技术(No.LGF20B070002)
  • 作者
  • 单位
  • 姜理英
  • 浙江工业大学环境学院, 杭州 310032
  • 张瑜芬
  • 浙江工业大学环境学院, 杭州 310032
  • 胡俊
  • 浙江工业大学环境学院, 杭州 310032
  • 姚志伟
  • 浙江工业大学环境学院, 杭州 310032
  • 黄武
  • 浙江工业大学环境学院, 杭州 310032
  • 汤露
  • 浙江工业大学环境学院, 杭州 310032
  • 摘要:以TiO2为载体,采用共沉淀法制备了3种双金属催化剂(Co-Mn/TiO2、Ce-Mn/TiO2和Nb-Mn/TiO2),与低温等离子体(NTP)协同对氯苯进行降解,并通过XRD、SEM、TEM、BET、XPS、H2-TPR和O2-TPD手段表征其物化性质,以阐明不同催化剂对氯苯的等离子体催化降解差异.结果显示,与单独的NTP相比,双金属催化剂耦合NTP可显著提高氯苯的降解效率和矿化率,减少有毒副产物的产生.Co-Mn/TiO2的催化活性优于Ce-Mn/TiO2和Nb-Mn/TiO2,在氯苯初始浓度为300 mg·m-3,气体停留时间为2 s,放电电压为15 kV的工况条件下,Co-Mn/TiO2耦合的NTP系统对氯苯的降解效率和CO2选择性分别达78.14%和51.02%,其O3的排放浓度为211 mg·m-3.表征结果也验证了以上结论,3种催化剂的金属氧化物均在TiO2表面高度分散,催化剂的比表面积为51~64 m2·g-1.Co-Mn/TiO2催化剂表面的高Mn4+/Mn3+比和Oads含量呈现出更多的氧空位,增大了氧迁徙率,因而表现出最高的催化活性和催化氧化性能.研究表明,双金属锰基催化剂耦合NTP降解氯苯具有很好的应用前景.
  • Abstract:Bimetallic manganese-based catalysts (Co-Mn/TiO2, Ce-Mn/TiO2 and Nb-Mn/TiO2) were supported on TiO2 by co-precipitation method and combined with non-thermal plasma (NTP) catalytic degradation of chlorobenzene (CB). The physicochemical properties of the catalysts were characterized by XRD、SEM、TEM、BET、XPS、H2-TPR and O2-TPD to clarify the differences between the various catalysts during the plasma catalytic degradation of CB. The experimental results showed that the bimetallic catalysts combined with NTP significantly improved the CB removal efficiency and mineralization rate compared with the NTP alone. Meanwhile, it greatly reduced the production of poisonous by-products (O3 and NOx). Co-Mn/TiO2 exhibited better catalytic activity than Ce-Mn/TiO2 and Nb-Mn/TiO2 in the NTP-catalysis reactor. At the initial concentration of 300 mg·m-3, residence time of 2 s and discharge voltage of 15 kV, the degradation efficiency and CO2 selectivity were 78.14% and 51.02% respectively in the Co-Mn/TiO2 coupled NTP reactor, and the emissions of O3 reached the minimum of 211 mg·m-3. The characterization results also verified that the metal oxides were highly dispersed on the surface of TiO2 for the catalysts, and the specific surface area was 51~64 m2·g-1. The high Mn4+/Mn3+ ratio and Oads content on the surface of the Co-Mn/TiO2 catalyst presented more O-vacancies and increased the oxygen migration rate, exhibiting the highest catalytic activity and redox property. Therefore, bimetallic manganese-based catalyst combined with NTP has a good application prospect for the degradation of CB.

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