College of Pipeline and Civil Engineering, China University of Petroleum, 66 Changjiang West Road, Qingdao 266580, China.
College of Pipeline and Civil Engineering, China University of Petroleum, 66 Changjiang West Road, Qingdao 266580, China.
J Colloid Interface Sci. 2018 Oct 15;528:82-91. doi: 10.1016/j.jcis.2018.05.061. Epub 2018 May 22.
The poisoning effect of PbO and PbCl on CeO-TiO catalyst for selective catalytic reduction of NO with NH was investigated and compared. Both Pb species could deactivate the CeO-TiO catalyst and PbO had a stronger poisoning effect than PbCl. From the characterization results of BET, XRD, XPS, NH-TPD and H-TPR, it was concluded that the more serious deactivation by PbO could be ascribed to smaller BET surface area, fewer surface Ce and chemisorbed oxygen, stronger interaction between PbO and CeO-TiO catalyst, lower redox properties and surface acidity. The in situ DRIFT study results revealed that the NH-SCR reaction over CeO-TiO catalyst was governed by both E-R and L-H mechanisms, which wasn't changed over the Pb-poisoned samples. The greater loss of Brønsted acid sites attributed to fewer surface Ce and more serious inhibition of NO oxidation to NO due to fewer surface chemisorbed oxygen were two key factors responsible for more serious deactivation by PbO. Furthermore, the presence of Pb species inhibited the NH adsorption on the Lewis acid sites, aggravating the deactivation of CeO-TiO catalyst.
研究并比较了 PbO 和 PbCl 对 CeO-TiO 催化剂用于选择性催化还原 NO 与 NH 的毒化作用。两种 Pb 物种均会使 CeO-TiO 催化剂失活,且 PbO 的毒化作用强于 PbCl。通过 BET、XRD、XPS、NH-TPD 和 H-TPR 的表征结果得出,PbO 导致更严重的失活可归因于更小的 BET 表面积、更少的表面 Ce 和化学吸附氧、PbO 与 CeO-TiO 催化剂之间更强的相互作用、更低的氧化还原性能和表面酸度。原位 DRIFT 研究结果表明,CeO-TiO 催化剂上的 NH-SCR 反应受 E-R 和 L-H 两种机理控制,而在 Pb 中毒样品上并未发生改变。表面 Ce 减少导致的 Brønsted 酸位大量损失以及表面化学吸附氧减少导致的 NO 氧化为 NO 的抑制作用增强,是 PbO 导致更严重失活的两个关键因素。此外,Pb 物种的存在抑制了 NH 在 Lewis 酸位上的吸附,从而加剧了 CeO-TiO 催化剂的失活。