唐南,黄妍,李元元,赵永谦,周婷,张俊丰,杨柳春.水热法制备铁锰催化剂脱硝性能及抗水抗硫性能研究[J].分子催化,2018,32(3):240-248
水热法制备铁锰催化剂脱硝性能及抗水抗硫性能研究
Low Temperature Selective Catalytic Reduction of NO with NH3 over Fe-Mn Catalysts Prepared by Hydrothermal Method
投稿时间:2018-02-07  修订日期:2018-03-25
DOI:
中文关键词:  MnOx-FeOy催化剂  水热法  抗水抗硫  低温NH3-SCR
英文关键词:MnOx-FeOy  sulfur resistance  hydrothermal method  NH3-SCR at low temperature
基金项目:湖南省高校创新平台开放基金项目(14k094)
作者单位E-mail
唐南 湘潭大学 环境与资源学院, 环境工程与科学系, 湖南 湘潭 411105  
黄妍 湘潭大学 环境与资源学院, 环境工程与科学系, 湖南 湘潭 411105 xtuhy@163.com 
李元元 湘潭大学 环境与资源学院, 环境工程与科学系, 湖南 湘潭 411105  
赵永谦 湘潭大学 环境与资源学院, 环境工程与科学系, 湖南 湘潭 411105  
周婷 湘潭大学 环境与资源学院, 环境工程与科学系, 湖南 湘潭 411105  
张俊丰 湘潭大学 环境与资源学院, 环境工程与科学系, 湖南 湘潭 411105  
杨柳春 湘潭大学 环境与资源学院, 环境工程与科学系, 湖南 湘潭 411105  
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中文摘要:
      采用水热法制备了MnOx-FeOy催化剂,在固定床模拟燃煤烟气气氛下考察其脱硝活性,并研究催化剂的抗水抗硫性能;采用XRD、BET、TEM、TG、XPS和H2-TPR技术对催化剂进行了表征.结果表明,一步水热法制备的MnOx-FeOy(Fe/(Fe+Mn)=0.5)催化剂,在80℃时NOx脱除率为90%,120℃脱硝效率达到99%.表征发现一步水热法合成的催化剂Mn和Fe之间存在较强的相互作用,Fe的掺杂可降低锰的起始还原温度,促进低温NH3-SCR反应.且其较大的比表面积以及较低的晶化程度使其具有较高的催化NOx活性.采用液相沉积-两步水热法制备的催化剂Fe/(Fe+Mn)=0.5HT在温度区间为150~250℃内,NOx脱除效率达到98%以上,同时该催化剂表现出较优的抗水抗硫性能,10% H2O和0.6% SO2同时作用8 h,NO转化率仍维持在73%左右,优于一步水热法合成的催化剂,且经500℃活化再生后,催化剂活性可基本恢复.这可能是由于Fe/(Fe+Mn)=0.5HT催化剂中,FeOy分散在MnOx表面,减少了硫酸铵盐和硫酸锰的沉积,提高了催化剂抗硫抗水性能.
英文摘要:
      MnOx-FeOy catalysts were synthesized using hydrothermal method and then developed as catalysts for the low temperature selective catalytic reduction(SCR) of NO with NH3, in a fixed bed simulated coal-burning atmosphere. Although the activity of MnOx-FeOy catalyst was suppressed in the presence of H2O and SO2. The catalysts were characterized by XRD, BET, TEM, TG and H2-TPR techniques. The NOx removal rate of the catalyst prepared by one step hydrothermal method reached 90% at the temperature of 80℃ and 99% at 120℃. It is found that there is a strong interaction between the catalyst Mn and Fe synthesized by one step hydrothermal method. The doping of Fe can reduce the initial reduction temperature of manganese and promote the NH3-SCR reaction at low temperature. And its large specific surface area and low crystallization degree make it have high NH3-SCR activity in the low temperature. The catalyst Fe/(Fe+ Mn)=0.5HT was prepared by two step hydrothermal method. It's NOx conversion reached more than 98% at the temperature of 150~250℃, although the catalyst shows better water and sulfur resistance. In the presence of 10% H2O and 0.6% SO2 the NOx conversion was more than 73%, when the Fe/(Fe+ Mn)=0.5 catalyst drop to 65%. This may be due to the FeOy deposition on the surface of MnOx. This structure may reduce the deposition of ammonium sulfate and ferric sulfate on the catalyst. Addition, the effects of different activation temperatures on the activity of the catalyst were studied. When the regeneration temperature is 500℃, the catalytic activity of Fe/(Fe +Mn)=0.5HT catalyst can be basically restored.
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