Key Laboratory of Biomass Chemical Engineering of Ministry of Education, Institute of Industrial Ecology and Environment, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.
Key Laboratory of Organosilicon Chemistry and Material Technology, Ministry of Education, College of Material, Chemistry and Chemical Engineering, Hangzhou Normal University, Hangzhou 311121, Zhejiang, P. R. China.
ACS Appl Mater Interfaces. 2023 Apr 12;15(14):17834-17847. doi: 10.1021/acsami.3c00212. Epub 2023 Mar 31.
The development of selective catalytic reduction catalysts by NH(NH-SCR) with excellent low-temperature activity and a wide temperature window is highly demanded but is still very challenging for the elimination of NO emission from vehicle exhaust. Herein, a series of sulfated modified iron-cerium composite oxide FeCeO-S catalysts were synthesized. Among them, the FeCeO-S catalyst achieved the highest NO conversion of more than 80% at temperatures of 175-375 °C under a gas hourly space velocity of 100000 h. Sulfation formed a large amount of sulfate on the surface of the catalyst and provided rich Brønsted acid sites, thus enhancing its NH adsorption capacity and improving the overall NO conversion efficiency. The introduction of Ce is the main determining factor in regulating the low-temperature activity of the catalyst by modulating its redox ability. Further investigation found that there is a strong interaction between Fe and Ce, which changed the electron density around the Fe ions in the FeCeO-S catalyst. This weakened the strength of the Fe-O bond and improved the lattice oxygen mobility of the catalyst. During the reaction, the iron-cerium composite oxide catalyst showed higher surface lattice oxygen activity and a faster replenishment rate of bulk lattice oxygen. This significantly improved the adsorption and activation of NO species and the activation of NH species on the catalyst surface, thus leading to the superior low-temperature activity of the catalyst.
本文采用 NH(NH-SCR)技术,开发了具有优异低温活性和较宽温度窗口的选择性催化还原催化剂,用于消除汽车尾气中的 NO 排放。本研究合成了一系列硫酸化改性的铁铈复合氧化物 FeCeO-S 催化剂。其中,在空速为 100000 h 的条件下,FeCeO-S 催化剂在 175-375°C 的温度范围内,NO 转化率超过 80%。硫酸化在催化剂表面形成了大量的硫酸盐,提供了丰富的 Brønsted 酸位,从而增强了其 NH 吸附能力,提高了整体 NO 转化效率。Ce 的引入是通过调节其氧化还原能力来调节催化剂低温活性的主要决定因素。进一步的研究发现,Fe 和 Ce 之间存在强烈的相互作用,改变了 FeCeO-S 催化剂中 Fe 离子周围的电子密度。这削弱了 Fe-O 键的强度,提高了催化剂的晶格氧迁移率。在反应过程中,铁铈复合氧化物催化剂表现出更高的表面晶格氧活性和更快的体相晶格氧补充速率。这显著改善了 NO 物种在催化剂表面的吸附和活化以及 NH 物种的活化,从而提高了催化剂的低温活性。