Chen Zhiqiang, Wang Hang, Zhang Xinjia, Wu Mei, Qu Hongxia
School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China; Faculty of Chemical Engineering, Huaiyin Institute of Technology, Huai'an 223003, China.
School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
J Hazard Mater. 2024 Sep 15;477:135268. doi: 10.1016/j.jhazmat.2024.135268. Epub 2024 Jul 20.
Although small pore Cu-SSZ-13 catalysts have been successful as commercial catalysts for controlling NO emissions from mobile sources, the challenges of high light-off temperature, SO tolerance and hydrothermal stability still need to be addressed. Here, we synthesized a multifunctional core-shell catalyst with Cu-SSZ-13 as the core phase and Ce-MnO supported Mesoporous-silica (Meso-SiO) as the shell phase via self-assembly and impregnation. The core-shell catalyst exhibited excellent low-temperature activity, SO tolerance and hydrothermal stability compared to the Cu-SSZ-13. The Ce-MnO species dispersed in the shell are found to enhance both the acidic and oxidative properties of the core-shell catalyst. More critically, these species can rapidly activate NO and oxidize it to NO, which allows the NH-SCR reaction on the core-shell catalyst to be initiated in the shell phase. Meanwhile, Ce-MnO species can react preferentially with SO as sacrifice components, effectively avoiding the sulfur inactivation of the copper active sites. Furthermore, the hydrophobic Meso-SiO shell provides an important barrier for the core phase, which reduces the loss of active species, acid sites and framework Al of the aged core-shell catalyst and mitigates the collapse of the zeolite framework. This work provides a new strategy for the design of novel and efficient NH-SCR catalysts.
尽管小孔径的Cu-SSZ-13催化剂作为控制移动源NO排放的商业催化剂已取得成功,但高光起燃温度、耐SO性能和水热稳定性等挑战仍需解决。在此,我们通过自组装和浸渍法合成了一种以Cu-SSZ-13为核相、Ce-MnO负载的介孔二氧化硅(Meso-SiO)为壳相的多功能核壳催化剂。与Cu-SSZ-13相比,该核壳催化剂表现出优异的低温活性、耐SO性能和水热稳定性。发现分散在壳层中的Ce-MnO物种增强了核壳催化剂的酸性和氧化性能。更关键的是,这些物种能快速活化NO并将其氧化为NO₂,这使得核壳催化剂上的NH-SCR反应能在壳层相中引发。同时,Ce-MnO物种可作为牺牲组分优先与SO₂反应,有效避免铜活性位点的硫失活。此外,疏水的Meso-SiO壳层为核相提供了重要屏障,减少了老化核壳催化剂活性物种、酸性位点和骨架Al的损失,并减轻了沸石骨架的坍塌。这项工作为设计新型高效的NH-SCR催化剂提供了新策略。