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工程科学与技术:2019,51(5):185-191
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Sn的掺杂对Ce-Mn/AC催化剂脱硝活性及抗硫性能的影响
(1.西南科技大学 环境与资源学院, 四川 绵阳 621010;2.国家烟气脱硫工程技术中心, 四川 成都 610065)
Effect of Sn Doping on Denitrification and Sulfur Resistance Performance of Ce-Mn/AC Catalyst
(1.Inst. of Environment and Resource, Southwest Univ. of Sci. and Technol., Mianyang 621010, China;2.National Eng. Research Center for Flue Gas Desulfurization, Chengdu 610065, China)
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投稿时间:2018-07-27    修订日期:2019-05-21
中文摘要: 为实现低温脱硝催化剂的工程化应用,研究如何进一步提高其活性和抗硫性非常必要。以活性炭为载体负载Ce-Mn制备了Ce-Mn/AC催化剂,采用Sn对催化剂进行掺杂改性,在考察Sn掺杂对催化剂结构性能影响的基础上,探讨和分析了结构性能变化对催化剂低温脱硝活性和抗硫性能的影响。采用XRD、XPS、N2吸附-脱附、NH3-TPD和H2-TPR等技术分别对催化剂的晶相结构、表面元素组成及化学位、结构性质、表面酸性和氧化还原性能进行了表征分析,并在固定床反应器上对催化剂的脱硝活性和抗硫性能进行了测试。结果表明:Sn的掺杂显著影响了催化剂的结构和性能,掺杂Sn后催化剂的结晶度增加,比表面积下降,活性组分的分散性降低;表面吸附氧和Ce3+比例下降,氧化还原性能降低;表面中强酸位数量下降,强酸位数量增加;催化剂的低温活性降低,抗硫性能有所提高。当Sn的掺杂量由0增加至1.5%时,催化剂对NO的起燃温度升高了135 ℃,且在整个反应温度区间内对NO的转化率降低了20%~40%,Sn掺杂量为0.5%的催化剂在150 ℃、100 μL/L含硫气氛中反应340 min后活性下降13%,降幅明显低于未掺杂Sn的催化剂,在210 ℃含硫气氛中的活性则随着反应时间的增加略有上升。催化剂低温活性的降低与其氧化还原性能的下降和活性组分的分散性降低有关,抗硫性能的提高则与表面酸性的提高有关。
中文关键词: 活性炭  催化剂  Sn掺杂  性能
Abstract:To achieve the engineering application of the low temperature denitration catalyst, it is necessary to study how to futher improve its activity and sulfur resistance. Activated carbon supported Ce-Mn catalyst with Sn doping was prepared. The effect of Sn on the structure and properties of catalyst was studied. The influence of structural property change on denitration performance and sulfur resistance of catalyst was studied. The crystalline phase structure, surface element composition, texture property, surface acidity and redox property of catalyst were characterized by means of XRD, XPS, N2 adsorption-desorption, NH3-TPD and H2-TPR techniques respectively. The activity and sulfur-resistance of catalyst for NH3 selective catalytic reduction was investigated in fixed bed reactor. The result showed that the structure and properties of catalyst was significantly affected by the doping of Sn. The doped Sn increased the crystallinity and reduced the specific surface area which led to decreased dispersity of active components. The reduction of adsorption oxygen and Ce3+ content was also reduced which induced the decline of redox performance. The number of medium-strong acid sites decreased while strong acid sites increased. The low temperature activity of the catalyst reduced, but the sulfur resistance was improved significantly. With the increase of Sn content from 0 to 1.5%, the light-off temperature for the conversion of NO raised 135 ℃, the NO conversion descended 20%~40% in whole range of test temperature. The activity of catalyst with 0.5% Sn doping was only decreased 13% after reaction 340 minutes at 150 ℃ and 100 μL/L SO2, which was significantly lower than catalyst without Sn. While at 210 ℃, the activity increased slightly with increase of reaction time. The reduction of low temperature activity of the catalyst was related to the decrease of redox property and dispersity of the active component, while the improvement of sulfur resistance was related to the increase of surface acidity.
文章编号:201800838     中图分类号:O643    文献标志码:
基金项目:四川省教育厅项目(17zd1145)
作者简介:黄利华(1979-),女,讲师,博士.研究方向:大气污染控制.E-mail:247860084@qq.com
引用文本:
黄利华,李雪,华坚.Sn的掺杂对Ce-Mn/AC催化剂脱硝活性及抗硫性能的影响[J].工程科学与技术,2019,51(5):185-191.
HUANG Lihua,LI Xue,HUA Jian.Effect of Sn Doping on Denitrification and Sulfur Resistance Performance of Ce-Mn/AC Catalyst[J].Advanced Engineering Sciences,2019,51(5):185-191.