Enhanced NH3-SCR performance of high-silica MER zeolite via template synthesis

IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Fuel Pub Date : 2025-02-28 DOI:10.1016/j.fuel.2025.134818
Yanhua Wang , Xiaoning Ren , Kaixiang Li , Yuankai Shao , Yang Zhou , Minru Zhao , Caixia Liu , Yatao Liu , Xi Liu , Anqi Dong , Hanming Wu , Maoxuan Wang , Lingwei Meng , Wang Zhang , Zhenguo Li , Qingling Liu
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Abstract

Amid increasingly stringent regulations on NOx emissions from diesel vehicles, Cu-based zeolite catalysts for ammonia selective catalytic reduction (NH3-SCR) are considered among the most effective solutions. MER zeolite, featuring a three-dimensional (3D) topology with 8-membered ring (8 MR) micropores, is typically Al-rich (Si/Al < 3) in conventional template-free synthesis. In this study, hierarchical O-MER zeolite with a higher Si/Al ratio (6.01) was efficiently synthesized using N, N-1, 1, 2, 6-tetramethylpiperidine as an organic template via inter-zeolite conversion over a crystallization period of 7–72 h. Compared to C-MER zeolite synthesized template-free, the Cu-based MER zeolite exhibited significantly enhanced NH3-SCR catalytic performance, achieving over 90 % NOx conversion within the 220–550 °C range for the fresh sample. Even after hydrothermal aging at 750 °C for 16 h, the sample maintained over 80 % NOx conversion between 250 and 550 °C. Comprehensive characterization revealed that hydrothermal aging partially degraded the crystalline structure of O-MER zeolite, notably reducing the number of acid sites, particularly Z-[Cu2+(OH)]+, which decreased NO activation and storage, thereby impacting low-temperature activity. The sustainable synthesis of MER zeolite and its robust catalytic performance present promising candidates for the future development of efficient and cost-effective SCR catalysts.

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模板合成法提高高硅MER分子筛NH3-SCR性能
随着柴油车氮氧化物排放法规的日益严格,铜基沸石催化剂用于氨选择性催化还原(NH3-SCR)被认为是最有效的解决方案之一。MER沸石具有三维(3D)拓扑结构,具有8元环(8mr)微孔,是典型的富Al (Si/Al <;3)传统的无模板合成。在本研究中,以N, N- 1,1,2,6 -四甲基哌替啶为有机模板,通过7-72 h的沸石间转化,高效地合成了Si/Al比(6.01)更高的O-MER分子筛。与无模板合成的C-MER分子筛相比,cu基MER分子筛表现出显著增强的NH3-SCR催化性能,在220-550℃范围内,新鲜样品的NOx转化率达到90%以上。即使在750℃水热时效16 h后,样品在250 ~ 550℃之间仍保持80%以上的NOx转化率。综合表征表明,水热老化使O-MER沸石的晶体结构部分降解,酸位数量明显减少,尤其是Z-[Cu2+(OH)−]+,降低了NO的活化和储存,从而影响了低温活性。MER沸石的可持续合成及其强大的催化性能为未来开发高效、经济的SCR催化剂提供了有希望的候选物。
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来源期刊
Fuel
Fuel 工程技术-工程:化工
CiteScore
12.80
自引率
20.30%
发文量
3506
审稿时长
64 days
期刊介绍: The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.
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