A superior cerium-tungsten bimetal oxide catalyst with flower-like structure for selective catalytic reduction of NO by NH3

催化作用 选择性催化还原 材料科学 双金属 氧化铈 氧化钨 氧化物 还原(数学) 无机化学 化学 冶金 有机化学 几何学 数学
作者
Xiaoxiang Wang,Heyao Ma,Beilei Li,Yaqing Wang,Shihan Zhang,Wei Li,Sujing Li
出处
期刊:Chemical Engineering Journal [Elsevier]
卷期号:435: 134892-134892 被引量:30
标识
DOI:10.1016/j.cej.2022.134892
摘要

• 0.1%WO 3 /CeO 2 (f) with flower-like morphology exhibited a wonderful NH 3 -SCR performance. • W loading strengthened the acidity while the structure of CeO 2 optimized the reducibility. • A strong interaction existed between surface WO x species and CeO 2 support. • NH 3 oxidization/deformation species could react with the gaseous or adsorbed NO x . • Bridged nitrates participated in the reaction via a L-H route over 0.1%WO 3 /CeO 2 (f). A novel flower-like 0.1%WO 3 /CeO 2 (f) catalyst with high-efficiency was fabricated for the selective reduction of NO x by NH 3 . In contrast to traditional WO 3 /CeO 2 , this catalyst exhibited a significant SCR performance of 90% NO x conversion and 95% N 2 selectivity within a wide temperature range of 175–450 °C and great H 2 O and/or SO 2 resistance under a high GHSV of 177,000 h −1 . A variety of analytical techniques including SEM, XRD, XPS, NH 3 -TPD, H 2 -TPR and in situ DRIFTS-MS were employed for the catalysts characterization to fully understand the reaction mechanism over WO 3 /CeO 2 catalysts. It was found that the flower-like structure promoted a more uniform dispersion of tungsten species on the support and a stronger interaction between WO 3 and CeO 2 , thereby increasing the acid sites and surface vacancies. Moreover, more chemical active oxygen and trivalent cerium species were presented on 0.1% WO 3 /CeO 2 (f). In situ DRIFTS-MS and H 2 -TPR revealed that the reducibility was optimized for 0.1% WO 3 /CeO 2 (f). Then NH 3 oxidation species could react with gaseous or adsorbed NO x during Eley-Rideal (E-R) pathway for 0.1%WO 3 /CeO 2 (f) at a high temperature (300 °C). Meanwhile, NO x was reduced into more active bridged nitrates participating in the reaction via Langmuir-Hinshelwood (L-H) route, contributing to its superior deNO x performance. In comparison, the formation of inert adsorbed NH 3 oxidization/deformation species and bridged nitrates suppressed the SCR reaction over 0.1%WO 3 /CeO 2 , resulting in its inferior deNO x activity. This study not only provides a new strategy for developing high-efficiency ceria supported NH 3 -SCR catalyst, but also lays a foundation for investigating the reaction mechanism of cerium-based catalyst for further practical applications.
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