School of Material Science and Engineering, Shanghai University, Shanghai 200072, China.
Nanoscale. 2013 Oct 7;5(19):9199-207. doi: 10.1039/c3nr02631k. Epub 2013 Aug 9.
Nanoflaky MnO(x) on carbon nanotubes (nf-MnO(x)@CNTs) was in situ synthesized by a facile chemical bath deposition route for low-temperature selective catalytic reduction (SCR) of NO with NH₃. This catalyst was mainly characterized by the techniques of X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), N₂ adsorption-desorption analysis, X-ray photoelectron spectroscopy (XPS), H₂ temperature-programmed reduction (H₂-TPR) and NH₃ temperature-programmed desorption (NH₃-TPD). The SEM, TEM, XRD results and N₂ adsorption-desorption analysis indicated that the CNTs were surrounded by nanoflaky MnO(x) and the obtained catalyst exhibited a large surface area as well. Compared with the MnO(x)/CNT and MnO(x)/TiO₂ catalysts prepared by an impregnation method, the nf-MnO(x)@CNTs presented better NH₃-SCR activity at low temperature and a more extensive operating temperature window. The XPS results showed that a higher atomic concentration of Mn(4+) and more chemisorbed oxygen species existed on the surface of CNTs for nf-MnO(x)@CNTs. The H₂-TPR and NH₃-TPD results demonstrated that the nf-MnO(x)@CNTs possessed stronger reducing ability, more acid sites and stronger acid strength than the other two catalysts. Based on the above mentioned favourable properties, the nf-MnO(x)@CNT catalyst has an excellent performance in the low-temperature SCR of NO to N₂ with NH₃. In addition, the nf-MnO(x)@CNT catalyst also presented favourable stability and H₂O resistance.
采用简便的化学浴沉积法原位合成了碳纳米管负载纳米片状 MnO(x)(nf-MnO(x)@CNTs),用于 NH₃ 低温选择性催化还原(SCR)NO。该催化剂主要采用 X 射线衍射(XRD)、透射电子显微镜(TEM)、扫描电子显微镜(SEM)、N₂吸附-脱附分析、X 射线光电子能谱(XPS)、H₂程序升温还原(H₂-TPR)和 NH₃ 程序升温脱附(NH₃-TPD)等技术进行了表征。SEM、TEM、XRD 结果和 N₂吸附-脱附分析表明,CNTs 被纳米片状 MnO(x)包围,所得到的催化剂具有较大的比表面积。与浸渍法制备的 MnO(x)/CNT 和 MnO(x)/TiO₂ 催化剂相比,nf-MnO(x)@CNTs 在低温下表现出更好的 NH₃-SCR 活性和更宽的操作温度窗口。XPS 结果表明,nf-MnO(x)@CNTs 表面存在更高的 Mn(4+)原子浓度和更多的化学吸附氧物种。H₂-TPR 和 NH₃-TPD 结果表明,nf-MnO(x)@CNTs 具有比其他两种催化剂更强的还原能力、更多的酸位和更强的酸强度。基于上述有利性质,nf-MnO(x)@CNT 催化剂在 NH₃ 低温 SCR 脱硝中具有优异的性能。此外,nf-MnO(x)@CNT 催化剂还表现出良好的稳定性和抗 H₂O 能力。