A superior cerium-tungsten bimetal oxide catalyst with flower-like structure for selective catalytic reduction of NOx by NH3

被引:31
|
作者
Wang, Xiaoxiang [1 ]
Ma, Heyao [1 ]
Li, Beilei [1 ]
Wang, Yaqing [1 ]
Zhang, Shihan [2 ]
Li, Wei [1 ]
Li, Sujing [1 ]
机构
[1] Zhejiang Univ, Coll Chem & Biol Engn, Inst Ind Ecol & Environm, Key Lab Biomass Chem Engn,Minist Educ, Hangzhou 310027, Peoples R China
[2] Zhejiang Univ Technol, Coll Environm, Hangzhou 310014, Peoples R China
基金
中国国家自然科学基金;
关键词
Tungsten-cerium catalyst; NH3-SCR; Flower-like structure; Oxidizability; Reducibility; ALKALI RESISTANCE; ACTIVATED CARBON; CEO2; CATALYST; SCR CATALYST; NH3-SCR; IR; PERFORMANCE; MECHANISM; IDENTIFICATION; REGENERATION;
D O I
10.1016/j.cej.2022.134892
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
A novel flower-like 0.1%WO3/CeO2(f) catalyst with high-efficiency was fabricated for the selective reduction of NOx by NH3. In contrast to traditional WO3/CeO2, this catalyst exhibited a significant SCR performance of 90% NOx conversion and 95% N2 selectivity within a wide temperature range of 175-450.C and great H2O and/or SO2 resistance under a high GHSV of 177,000 h 1. A variety of analytical techniques including SEM, XRD, XPS, NH3-TPD, H2-TPR and in situ DRIFTS-MS were employed for the catalysts characterization to fully understand the reaction mechanism over WO3/CeO2 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 WO3 and CeO2, thereby increasing the acid sites and surface vacancies. Moreover, more chemical active oxygen and trivalent cerium species were presented on 0.1% WO3/CeO2(f). In situ DRIFTS-MS and H2-TPR revealed that the reducibility was optimized for 0.1% WO3/CeO2(f). Then NH3 oxidation species could react with gaseous or adsorbed NOx during Eley-Rideal (E-R) pathway for 0.1%WO3/CeO2(f) at a high temperature (300. C). Meanwhile, NOx was reduced into more active bridged nitrates participating in the reaction via Langmuir-Hinshelwood (L-H) route, contributing to its superior deNOx performance. In comparison, the formation of inert adsorbed NH3 oxidization/ deformation species and bridged nitrates suppressed the SCR reaction over 0.1%WO3/CeO2, resulting in its inferior deNOx activity. This study not only provides a new strategy for developing high-efficiency ceria supported NH3-SCR catalyst, but also lays a foundation for investigating the reaction mechanism of cerium-based catalyst for further practical applications.
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页数:12
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