Faculty of Chemistry, Jagiellonian University in Kraków, Gronostajowa 2, 30-387 Kraków, Poland.
Institute of Geological Sciences, Jagiellonian University in Kraków, Gronostajowa 3a, 30-387 Kraków, Poland.
Molecules. 2020 Nov 30;25(23):5651. doi: 10.3390/molecules25235651.
Spherical MCM-41 with various copper and iron loadings was prepared by surfactant directed co-condensation method. The obtained samples were characterized with respect to their structure (X-ray diffraction, XRD), texture (N sorption), morphology (scanning electron microscopy, SEM), chemical composition (inductively coupled plasma optical emission spectrometry, ICP-OES), surface acidity (temperature programmed desorption of ammonia, NH-TPD), form, and aggregation of iron and copper species (diffuse reflectance UV-Vis spectroscopy, UV-Vis DRS) as well as their reducibility (temperature programmed reduction with hydrogen, H-TPR). The spherical MCM-41 samples modified with transition metals were tested as catalysts of selective catalytic reduction of NO with ammonia (NH-SCR). Copper containing catalysts presented high catalytic activity at low-temperature NH-SCR with a very high selectivity to nitrogen, which is desired reaction products. Similar results were obtained for iron containing catalysts, however in this case the loadings and forms of iron incorporated into silica samples very strongly influenced catalytic performance of the studied samples. The efficiency of the NH-SCR process at higher temperatures was significantly limited by the side reaction of direct ammonia oxidation. The reactivity of ammonia molecules chemisorbed on the catalysts surface in NO reduction (NH-SCR) and their selective oxidation (NH-SCO) was verified by temperature-programmed surface reactions.
采用表面活性剂导向共缩聚方法制备了具有不同铜和铁负载量的球形 MCM-41。对所得样品进行了结构(X 射线衍射,XRD)、织构(N 吸附)、形貌(扫描电子显微镜,SEM)、化学组成(电感耦合等离子体发射光谱,ICP-OES)、表面酸度(氨程序升温脱附,NH-TPD)、形态和铁和铜物种的聚集(漫反射紫外可见光谱,UV-Vis DRS)以及它们的还原性(用氢气程序升温还原,H-TPR)等方面的特征。将过渡金属改性的球形 MCM-41 样品用作氨选择性催化还原 NO 的催化剂(NH-SCR)。含铜的催化剂在低温 NH-SCR 中表现出高催化活性,对氮气具有很高的选择性,这是所需的反应产物。含铁的催化剂也得到了类似的结果,但是在这种情况下,铁的负载量和形式强烈影响了研究样品的催化性能。在较高温度下 NH-SCR 过程的效率受到直接氨氧化副反应的显著限制。通过程序升温表面反应验证了催化剂表面吸附的氨分子在 NO 还原(NH-SCR)和选择性氧化(NH-SCO)中的反应性。