Energy Research Institute, Nanjing Institute of Technology, Nanjing 211167, China.
Institute of Catalysis, Zhejiang University, Hangzhou 310028, China.
J Environ Sci (China). 2021 Feb;100:306-316. doi: 10.1016/j.jes.2020.08.003. Epub 2020 Aug 14.
Series of Fe/Cu-SSZ-13 catalysts with different Fe loading content were synthesized by simple one-pot strategy. The obtained catalysts were subjected to selective catalytic reduction (SCR) of NO with NH and were characterized by various techniques. The results show that Fe/Cu-SSZ-13 catalyst with proper Fe content exhibits excellent catalytic activity with widest operation temperature window from 160 to 580°C, excellent hydrothermal stability as well as good resistance to sulfur poisoning when compared with Cu-SSZ-13, signifying its great potential for practical applications. Further characterizations reveal that the synthesized Fe/Cu-SSZ-13 catalysts present typical chabazite (CHA) structure with good crystallinity, while isolated Cu and monomeric Fe are revealed as the predominant copper and iron species. At low temperatures, isolated Cu species act as primary active sites for SCR reaction, while monomeric Fe species provide sufficient active sites for sustain the SCR activity at high temperature. Moreover, Fe over doping would lead to the damage of zeolite structure, destruction of isolated Cu site, as well as the formation of highly oxidizing FeO, thus causing deterioration of catalytic performances.
采用简单的一锅法合成了一系列不同铁负载量的 Fe/Cu-SSZ-13 催化剂。通过各种技术对所得催化剂进行了选择性催化还原(SCR)NO 与 NH 的反应,并进行了表征。结果表明,与 Cu-SSZ-13 相比,具有适当铁含量的 Fe/Cu-SSZ-13 催化剂具有优异的催化活性,操作温度窗口最宽,为 160 至 580°C,具有出色的热稳定性以及良好的抗硫中毒能力,表明其在实际应用中具有很大的潜力。进一步的表征表明,合成的 Fe/Cu-SSZ-13 催化剂呈现出典型的菱沸石(CHA)结构,具有良好的结晶度,而孤立的 Cu 和单体 Fe 则被揭示为主要的铜和铁物种。在低温下,孤立的 Cu 物种作为 SCR 反应的主要活性位,而单体 Fe 物种则提供了足够的活性位,以维持高温下的 SCR 活性。此外,铁的过度掺杂会导致沸石结构的破坏、孤立 Cu 位的破坏以及强氧化性 FeO 的形成,从而导致催化性能的恶化。