Boosting low-temperature and high-temperature hydrothermal stability of Cu/SAPO-34 for NO removal via yttrium decoration

热液循环 催化作用 氮氧化物 材料科学 沸石 化学工程 水热合成 吸附 核化学 矿物学 无机化学 化学 物理化学 有机化学 燃烧 工程类 氧化物
作者
Lianyun Gao,Wenfeng Gao,Huimin Wang,Siyuan Xu,Xiaoyan Tian,Jinyan Cao,Jianjun Chen,Qiulin Zhang,Ping Ning,Jiming Hao
出处
期刊:Chemical Engineering Journal [Elsevier BV]
卷期号:455: 140520-140520 被引量:18
标识
DOI:10.1016/j.cej.2022.140520
摘要

Cu/SAPO-34 SCR catalysts have been widely investigated for NOx removal in past decades. However, the inferior hydrothermal stability of these catalysts greatly limited their industrial application. In this work, Cu/SAPO-34 docorated by yttrium (Y) were synthesized and the effects of Y on the low-temperature (L-T, 70 °C) and high-temperature (H-T, 850 °C) hydrothermal stability of Cu-SAPO-34 as well as the mechanisms were systematically studied at atomic-level. The results showed that Y imbedding slightly enhanced L-T hydrothermal stability but significantly improved H-T one of Cu-SAPO-34. Typically, even suffering from H-T hydrothermal aging at 850 °C for 10 h at 10 vol.%H2O, the Y modified Cu-SAPO-34 (Cu/Y-S-850) still presented relatively higher NOx conversion (80–100 %) at a wide temperature window of 225–450 °C than the reference one (Cu/S-850) (<40 %), which is superior to those of most reported CHA-based SCR catalysts. This promotion could be due to the fact that Y decoration can minimize the broken of Si-O-Al bonds and inhibit the collapse of the zeolite skeleton, which in turn kept an intact CHA structure and helped active Cu2+ species disperse well, thus exposing abundant active Cu2+ component during harsh aging. Additionally, numerous Brønsted and Lewis acid sites over the Y modified catalysts were almost maintained. From this way, NOx was adsorbed, activated, and conversed smoothly via both “L-H” and “E-R” mechanisms.
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