Yu Chenglong, Chen Feng, Dong Lifu, Liu Xiaoqing, Huang Bichun, Wang Xinnan, Zhong Shengbang
School of Environment and Energy, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou, 510006, People's Republic of China.
Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, South China University of Technology, Guangzhou Higher Education Mega Centre, Guangzhou, 510006, People's Republic of China.
Environ Sci Pollut Res Int. 2017 Mar;24(8):7499-7510. doi: 10.1007/s11356-017-8375-0. Epub 2017 Jan 23.
Manganese-rich MnSAPO-34 molecular sieves were prepared by one-pot synthesis method for NO abatement using the ammonia-selective catalytic reduction (NH-SCR) technology and characterized using ICP, BET, XRD, FE-SEM, H-TPR, NH-TPD, XPS, and DR UV-Vis analyses. The experimental results indicate that the Mn content and chemical state, as well as the surface acidity, of the MnSAPO-34 molecular sieves significantly enhance their DeNO efficiency at low temperatures (ca. 200-300 °C). The manganese-rich MnSAPO-34 was synthesized using a combination of triethylamine and diisopropylamine as the structural directing agents and high Mn loading (n(MnO)/n(PO) = 0.4). The resulting catalyst exhibits the highest activity among all of the samples with a NO conversion value of nearly 95% and a N selectivity that is higher than 90% at 220-400 °C. In addition, this catalyst presents higher NO conversion than the conventional VO-WO/TiO catalysts and other SAPO-based catalysts below 300 °C. Furthermore, the analytical results indicate that the manganese species in the catalyst are mainly in the form of a framework Mn(IV), which could play a significant role in the NH-SCR process as the specific active species. The results suggest that controlling the types and content of the organic amine templates and variations in the surface acidity of the catalysts may significantly enhance the SCR activity at lower temperatures.
采用一锅法合成了富锰MnSAPO-34分子筛,用于氨选择性催化还原(NH-SCR)技术脱除NO,并通过电感耦合等离子体发射光谱(ICP)、比表面积测定(BET)、X射线衍射(XRD)、场发射扫描电子显微镜(FE-SEM)、氢气程序升温还原(H-TPR)、氨气程序升温脱附(NH-TPD)、X射线光电子能谱(XPS)和漫反射紫外可见光谱(DR UV-Vis)分析对其进行了表征。实验结果表明,MnSAPO-34分子筛的锰含量、化学状态以及表面酸度显著提高了其在低温(约200-300℃)下的脱硝效率。以三乙胺和二异丙胺为结构导向剂,采用高锰负载量(n(MnO)/n(PO)=0.4)合成了富锰MnSAPO-34。所得催化剂在所有样品中表现出最高的活性,在220-400℃下NO转化率接近95%,N选择性高于90%。此外,该催化剂在300℃以下的NO转化率高于传统的VO-WO/TiO催化剂和其他基于SAPO的催化剂。此外,分析结果表明,催化剂中的锰物种主要以骨架Mn(IV)的形式存在,作为特定的活性物种,在NH-SCR过程中可能发挥重要作用。结果表明,控制有机胺模板的类型和含量以及催化剂表面酸度的变化可能显著提高低温下的SCR活性。