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Ce-Mn/TiO2吸附剂的脱汞性能及抗SO2特性
引用本文:吴响,段钰锋,姚婷,李娜,胡鹏,韦红旗,任少君.Ce-Mn/TiO2吸附剂的脱汞性能及抗SO2特性[J].中国环境科学,2019,39(6):2336-2343.
作者姓名:吴响  段钰锋  姚婷  李娜  胡鹏  韦红旗  任少君
作者单位:东南大学能源与环境学院, 能源热转换及其过程测控教育部重点实验室, 江苏 南京 210096
基金项目:国家重点研发计划(2016YFC0201105);国家自然科学基金(51876039,51676041)
摘    要:采用浸渍法制备Mn/TiO2(MT)、Ce/TiO2(CT)和Ce-Mn/TiO2(CMT)脱汞吸附剂,在固定床脱汞实验台上研究吸附剂的脱汞性能.结果表明,吸附温度为100~200℃时,3种吸附剂的脱汞性能均随温度的升高而增强;而在200~300℃范围内,脱汞效率均出现不同程度的降低.MT、CT及CMT吸附剂的脱汞效率在200℃时达到最高,分别为91%、58%和95%.MT和CT吸附剂的抗SO2性能较弱,在N2+6% O2+1000×10-6SO2烟气条件下,30min内脱汞效率均下降到50%,而CMT吸附剂在2h内仍能保持80%以上的脱汞效率,表明在MT中掺杂Ce不仅可以提高吸附剂的脱汞性能,还可以增强抗SO2性能.利用N2吸附/脱附、X射线衍射(XRD)、H2-程序升温还原(H2-TPR)和X射线光电子能谱(XPS)等方法对吸附剂的物理化学性质进行表征,并对吸附产物进行热重分析(TG)和程序升温脱附实验(TPD),阐明了CMT脱汞吸附剂的抗SO2特性机理.Ce的掺杂,提高了活性组分在吸附剂表面的分散度及Mn4+的比例;相比于MnO2,CeO2可优先与SO2反应,抑制了SO2对Mn4+的毒害作用,从而提高了抗硫性能.

关 键 词:    吸附剂  脱汞  抗硫能力  
收稿时间:2018-11-12

Mercury removal performance and SO2 resistance of Ce-Mn/TiO2 sorbent
WU Xiang,DUAN Yu-feng,YAO Ting,LI Na,HU Peng,WEI Hong-qi,REN Shao-jun.Mercury removal performance and SO2 resistance of Ce-Mn/TiO2 sorbent[J].China Environmental Science,2019,39(6):2336-2343.
Authors:WU Xiang  DUAN Yu-feng  YAO Ting  LI Na  HU Peng  WEI Hong-qi  REN Shao-jun
Institution:Key Laboratory of Energy Thermal Conversion and Control, Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, China
Abstract:Mn/TiO2 (MT), Ce/TiO2 (CT) and Ce-Mn/TiO2 (CMT) sorbents for mercury removal were prepared by the impregnation method. Mercury adsorption experiments were conducted on a fixed-bed reactor. The mercury removal performance of the three sorbents gradually increased with the increase of temperature in the range of 100~200℃. The maximum mercury capture efficiency of 91%, 58% and 95% were observed at 200℃ for MT, CT and CMT, respectively. The mercury removal efficiency decreased when the temperature was higher than 200℃. When MT and CT sorbents were exposed in the flue gas with N2+6%O2+1000×10-6SO2, the decrease of mercury removal efficiency to 50% within 30min was observed, indicating the weak SO2resistance of MT and CT. However, mercury removal efficiency of more than 80% was maintained by CMT within 2h. It revealed that Ce doping in MT not only improved the mercury removal performance, but also enhanced the SO2resistance. Physicochemical characteristics of the sorbents were analyzed by N2adsorption/desorption, X-ray diffraction (XRD), H2-temperature programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS). The spent sorbents were analyzed by thermogravimetric analysis (TG) and temperature programmed desorption (TPD) experiments. Based on the experimental and characterization results, the mechanism of SO2resistance of the CMT for mercury removal was interpreted. The doping of Ce improved the dispersion of active components on the sorbent surface and the ratio of Mn4+, which was favorable for mercury removal; Compared with MnO2, CeO2preferentially react with SO2, which inhibited the toxic effect on Mn4+, thus improving the SO2resistance.
Keywords:manganese  cerium  sorbent  Hg0 removal  SO2 resistance performance  
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