International Joint Laboratory of Catalytic Chemistry, Department of Chemistry, Research Center of Nano Science and Technology, College of Sciences, Shanghai University, Shanghai 200444, China.
State Key Laboratory of Marine Resource Utilization in South China Sea, School of Materials Science and Engineering, Hainan University, Haikou 570228, Hainan, China.
Environ Sci Technol. 2020 Oct 6;54(19):12752-12760. doi: 10.1021/acs.est.0c04911. Epub 2020 Sep 16.
Reducing the poisoning effect of alkali and heavy metals over ammonia selective catalytic reduction (NH-SCR) catalysts is still an intractable issue, as the presence of K and Pb in fly ash greatly hampers their catalytic activity by impairing the acidity and affecting the redox properties of the catalysts, leading to the reduction in the lifetime of SCR catalysts. To address this issue, we propose a novel self-protected antipoisoning mechanism by designing SO/TiO superacid supported CeO-SnO catalysts. Owing to the synergistic effect between CeO and SnO and the strong acidity originating from the SO/TiO superacid, the catalysts show superior catalytic activity over a wide temperature range (240-510 °C). Moreover, when K or/and Pb are deposited on SO/TiO catalysts, the bond effect between SO and Ti-O would be broken so that the sulfate in the bulk of SO/TiO superacid support would be induced to migrate to the surface to bond with K and Pb, thus prohibiting poisons from attacking the Ce-Sn active sites, and significantly boosting the resistance. Hopefully, this novel self-protection mechanism derived from the migration of sulfate in the SO/TiO superacid to resist alkali and heavy metals provides a new avenue for designing novel catalysts with outstanding resistance to alkali and heavy metals.
降低碱和重金属对氨选择性催化还原(NH-SCR)催化剂的毒害作用仍然是一个棘手的问题,因为飞灰中的 K 和 Pb 会通过损害酸度和影响催化剂的氧化还原性能来极大地阻碍其催化活性,从而缩短 SCR 催化剂的使用寿命。为了解决这个问题,我们提出了一种新颖的自保护抗中毒机制,通过设计 SO/TiO 超强酸负载的 CeO-SnO 催化剂。由于 CeO 和 SnO 之间的协同效应以及 SO/TiO 超强酸的强酸性,催化剂在很宽的温度范围内(240-510°C)表现出优异的催化活性。此外,当 K 或/和 Pb 沉积在 SO/TiO 催化剂上时,SO 和 Ti-O 之间的键合效应会被打破,从而导致 SO/TiO 超强酸载体中的硫酸盐会诱导迁移到表面与 K 和 Pb 键合,从而阻止毒物攻击 Ce-Sn 活性位,显著提高其抗毒性。希望这种源自 SO/TiO 超强酸中硫酸盐迁移的新型自保护机制能够抵抗碱和重金属,为设计具有优异抗碱和重金属性能的新型催化剂提供新途径。