DRIFT and DFT study of cerium addition on SO2 of Manganese-based Catalysts for low temperature SCR
DRIFT and DFT study of cerium addition on SO2 of Manganese-based Catalysts for low temperature SCR
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低温SCR锰基催化剂SO2添加铈的DRIFT和DFT研究
DOI：
10.1016/j.molcata.2016.05.013
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发表时间：
2016-09
期刊：
影响因子：
--
通讯作者：
Zhang Liangjing
中科院分区：
文献类型：
--
作者：
Wei Lu;Cui Suping;Guo Hongxia;Ma Xiaoyu;Zhang Liangjing
研究了Mn/TiO_2和Mn-Ce/TiO_2催化剂的SO_2中毒机理，揭示了铈的抗中毒作用。在SO2存在下，两种催化剂均失活，降低了NOx的脱除率，但Ce掺杂催化剂的抗硫性能明显提高。DRIFT和DFT结果表明，SO2首先吸附在锰端（刘易斯酸中心）形成硫酸盐，抑制了SCR反应中NH3的吸附.布朗斯台德酸中心的失活是由于亚硫酸氢盐的形成，亚硫酸氢盐可以与NH 4+反应形成NH 4 HSO 4。在Mn-Ce/TiO 2催化剂中，SO2以硫酸盐形式优先吸附在Ce原子上，缓解了催化剂主要活性中心（MnOx上的刘易斯酸中心和Broøsted酸中心）的硫酸化.此外，硫酸铈可以产生新的布朗斯台德酸中心，并有助于低温SCR过程。
The mechanisms of sulfur dioxide poisoning on Mn/TiO2and Mn-Ce/TiO2catalysts are studied and poisoning resistance effect of cerium is revealed. Both two kinds of catalysts were deactivated to reduce NOxremoval in the presence of SO2, however, the sulfur resistance performance of the Ce doping catalysts was obviously improved. From the result of DRIFT and DFT, SO2can first adsorb on the manganese-terminal (Lewis acid sites) to form sulfates, which inhibit the adsorption of NH3in the SCR reaction. Deactivation of Brønsted acid sites was due to the formation of bisulfite, which can react with NH4+form NH4HSO4. For the Mn-Ce/TiO2catalysts, SO2preferentially adsorbed on Ce atom as sulfate species, alleviating the sulfation of the main active sites (Lewis acid sites and Broøsted acid site on MnOx) under the effect of SO2. Furthermore, cerium sulfate can produce new Brønsted acid site and contribute to the low-temperature SCR processes.
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