Szymaszek-Wawryca Agnieszka, Summa Paulina, Duraczyńska Dorota, Díaz Urbano, Motak Monika
Faculty of Energy and Fuels, AGH University of Science and Technology, Al. Adama Mickiewicza 30, 30-059 Krakow, Poland.
Jerzy Haber Institute of Catalysis and Surface Chemistry, Polish Academy of Sciences, Ul. Niezapominajek 8, 30-239 Krakow, Poland.
Materials (Basel). 2022 Nov 8;15(22):7884. doi: 10.3390/ma15227884.
A series of clinoptilolite-supported catalysts, modified with hydrotalcite-like phase (HT) by co-precipitation, were prepared and tested in NH-SCR reactions. It was found that deposition of HT on clinoptilolite increased conversion of NO within 250-450 °C, and that the positive impact on the catalytic activity was independent of HT loading. The promoting effect of clinoptilolite was attributed to Brönsted acid sites present in the zeolite, which facilitated adsorption and accumulation of ammonia during the catalytic process. Concentration of NO in the post-reaction gas mixture reached its maximum at 300 °C and the by-product was most likely formed as a consequence of NHNO decomposition or side reaction of NH oxidation in the high-temperature region. The gradual elimination of nitrous oxide, noticed as the material with the highest concentration of hydrotalcite phase, was attributed to the abundance of oligomeric iron species and the superior textural parameters of the material. UV-Vis experiments performed on the calcined samples indicated that Fe sites of higher nuclearity were generated by thermal decomposition of the hydrotalcite phase during the catalytic reaction. Therefore, calcination of the materials prior to the catalytic tests was not required to obtain satisfactory overall catalytic performance in NO reductions.
通过共沉淀法制备了一系列用类水滑石相(HT)改性的斜发沸石负载型催化剂,并在NH-SCR反应中进行了测试。结果发现,HT沉积在斜发沸石上可提高250-450℃范围内NO的转化率,且对催化活性的积极影响与HT负载量无关。斜发沸石的促进作用归因于沸石中存在的布朗斯台德酸位,其在催化过程中促进了氨的吸附和积累。反应后气体混合物中NO的浓度在300℃时达到最大值,副产物很可能是由NHNO分解或高温区域NH氧化的副反应形成的。作为水滑石相浓度最高的材料,其氧化亚氮的逐渐消除归因于大量的低聚铁物种和该材料优异的织构参数。对煅烧样品进行的紫外-可见实验表明,在催化反应过程中,水滑石相的热分解产生了更高核数的铁位点。因此,在催化测试之前不需要对材料进行煅烧就能在NO还原中获得令人满意的整体催化性能。