Pang Chengkai, Zhuo Yuqun, Weng Qiyu, Zhu Zhenwu
Key Laboratory for Thermal Science and Power Engineering of Ministry of Education, Beijing Engineering Research Center for Ecological Restoration and Carbon Fixation of Saline-alkaline and Desert Land, Department of Thermal Engineering, Tsinghua University Beijing 100084 China
RSC Adv. 2018 Feb 6;8(11):6110-6119. doi: 10.1039/c7ra12350g. eCollection 2018 Feb 2.
The activity and hydrothermal stability of Cu/SAPO and Mn-2Cu/SAPO for low-temperature selective catalytic reduction of NO with ammonia were investigated. An ion-exchanged method was employed to synthesize Mn-2Cu/SAPO, which was characterized by N adsorption, ICP-AES, X-ray diffraction (XRD), NH-temperature programmed desorption (NH-TPD), NO oxidation, X-ray photoelectron spectrum (XPS), UV-vis, H-temperature programmed reduction (H-TPR) and diffuse reflectance infrared Fourier transform spectra (DRIFTS). 2Mn-2Cu/SAPO and 4Mn-2Cu/SAPO showed the best SCR activity, in that at 150 °C NO conversion reached 76% and N selectivity was above 95% for the samples. NO oxidation results showed that the 2Mn-2Cu/SAPO had the best NO oxidation activity and the BET surface area decreased as manganese loading increased. XRD results showed that the metal species was well dispersed. NH-TPD showed that the acid sites have no significant influence on the SCR activity of Mn-2Cu/SAPO. H-TPR patterns showed good redox capacity for Mn-2Cu/SAPO. UV-vis and H-TPR showed that the ratio of Mn to Mn increased as manganese loading increased. XPS spectra showed a significant amount of Mn and Mn species on the surface and addition of manganese increased the ratio of Cu. The promotion effect of manganese to 2Cu/SAPO comes from the generation of Mn and Mn species. Deduced from the DRIFTS spectra, the Elay-Rideal mechanism was effective on 4Mn-2Cu/SAPO.
研究了Cu/SAPO和Mn-2Cu/SAPO在低温下用氨选择性催化还原NO的活性和水热稳定性。采用离子交换法合成了Mn-2Cu/SAPO,并通过N吸附、ICP-AES、X射线衍射(XRD)、NH-程序升温脱附(NH-TPD)、NO氧化、X射线光电子能谱(XPS)、紫外可见光谱、H-程序升温还原(H-TPR)和漫反射红外傅里叶变换光谱(DRIFTS)对其进行了表征。2Mn-2Cu/SAPO和4Mn-2Cu/SAPO表现出最佳的SCR活性,在150℃时,样品的NO转化率达到76%,N选择性高于95%。NO氧化结果表明,2Mn-2Cu/SAPO具有最佳的NO氧化活性,且BET比表面积随锰负载量的增加而减小。XRD结果表明金属物种分散良好。NH-TPD表明酸性位点对Mn-2Cu/SAPO的SCR活性没有显著影响。H-TPR图谱表明Mn-2Cu/SAPO具有良好的氧化还原能力。紫外可见光谱和H-TPR表明,随着锰负载量的增加,Mn与Mn的比例增加。XPS光谱表明表面存在大量的Mn和Mn物种,锰的加入增加了Cu的比例。锰对2Cu/SAPO的促进作用源于Mn和Mn物种的生成。从DRIFTS光谱推断,Elay-Rideal机理对4Mn-2Cu/SAPO有效。