| Mn-Co/蜂窝陶瓷催化剂制备及催化臭氧化对苯二酚效能 |
| 摘要点击 1740 全文点击 596 投稿时间：2017-11-06 修订日期：2017-12-23 |
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| 中文关键词 涂覆法 催化臭氧化 对苯二酚 Mn-Co/CH催化剂 动力学 |
| 英文关键词 coating method catalytic ozonation hydroquinone Mn-Co/CH catalyst kinetics |
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| 中文摘要 |
| 为了提高金属催化剂的活性和使用寿命，以硝酸钴Co（NO3）2·6H2O和硝酸锰Mn（NO3）2作为前驱体，蜂窝陶瓷（ceramic honeycomb，CH）作为载体，采用涂覆法制备了4种不同质量比的Mn-Co/CH催化剂，通过XRD、N2-吸附/脱附、FESEM和XPS等方法分析了催化剂的结构，研究了催化剂的材料力学性能，建立了单独臭氧和催化臭氧化对苯二酚的反应动力学模型，考察了催化剂催化臭氧化的效能.结果表明，Mn1Co1/CH（Mn ∶Co=1 ∶1）催化剂的晶相主要以Mn3O4和CoO为主，具有较大的比表面积、孔容和孔径，分别达到190 m2·g-1、0.25 cm3·g-1和4.8 nm；Mn1Co1/CH催化剂的催化活性最高，对苯二酚和COD的去除率分别达到78%和54%.Mn-Co/CH催化剂的抗压缩强度大（15.89~16.94 MPa）.当添加叔丁醇时，对苯二酚去除率显著下降，·OH在Mn1Co1/CH催化臭氧化过程中起着重要的作用，催化臭氧化对苯二酚符合一级反应动力学模型.Mn-Co/CH催化剂用量少、催化效率高、使用寿命长，易于实现工业化. |
| 英文摘要 |
| In order to improve the activity and working life of metal catalysts in the heterogeneous catalytic ozonation of organic wastewater, four kinds of Mn-Co/ceramic honeycomb (CH) catalysts with different mass ratios of Mn and Co were prepared by coating method using cobalt nitrate hexahydrate [Co(NO3)2·6H2O] and manganese nitrate [Mn(NO3)2] as precursors, respectively, and CH as the carrier. The structure of the catalysts was analyzed via X-ray diffraction (XRD), N2 adsorption/desorption, field emission scanning electron microscopy (FESEM), and X-ray photoelectron spectroscopy (XPS). The mechanical properties of the catalysts were studied. The reaction kinetics model of O3 alone and catalytic ozonation of the hydroquinone were established and catalytic ozonation performance of catalysts was investigated. The results showed that the crystal phase of Mn0Co1/CH belonged to CoAl2O4 and that the crystal phase of the Mn-Co/CH catalyst (Mn1Co1, Mn2Co1, and Mn3Co1) mainly belonged to Mn3O4 and CoO. In particular, the Mn1Co1/CH catalyst had a large specific surface area of 190 m2·g-1, high pore volume of 0.25 cm3·g-1, and pore size of 4.8 nm. The highest catalytic activity was obtained when Mn∶Co was 1∶1 (Mn1Co1/CH catalyst). The catalytic activity of the Mn1Co1/CH catalyst was the highest, and removal efficiencies of hydroquinone and COD were 78% and 54%, respectively, using Mn1Co1/CH catalytic ozonation. The Mn-Co/CH catalyst had a high compressive strength (15.89-16.94 MPa). The degradation efficiency of hydroquinone decreased significantly after the addition of tert-butanol, which indicated that·OH played an important role in the Mn1Co1/CH catalytic ozonation. The catalytic ozonation process fitted the first-order kinetic model. The apparent rate constant k for O3 alone was only 0.0306. Furthermore, the Mn1Co1/CH catalyst had the highest rate, with an apparent rate constant k of 0.0535 min-1. The Mn-Co/CH catalyst was easy to industrialize owing to its lower consumption, excellent catalytic characteristics, and long working life. |
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