Mesoporous zeolite ZSM-5 confined Cu nanoclusters for efficient selective catalytic reduction of NOx by NH3

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2024-01-17 DOI:10.1016/j.apcatb.2024.123747

Sun Yuanyuan , Zhanyu Li , Xiaoxia Zhou , Guohui Li , Min Tan , Shuang Ao , Wei Sun , Hangrong Chen

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Abstract

Cu-based catalysts have been widely used in ammonia-selective catalytic reduction (NH₃-SCR) of NO_x for their excellent low temperature denitration performance. However, the aggregation of Cu species has been a troubling problem in catalyst design. Herein, spherical zeolite ZSM-5 confined Cu nanoclusters Cu@ZSM-5 has been successfully constructed via in-situ self-assembly process. It exhibits high specific surface area (373 m²g⁻¹), higher concentration of Cu⁺, rich oxygen vacancies and more acid sites compared with Cu/ZSM-5. The results indicate that strong acid sites of carrier could improve high-temperature catalytic activity, and Cu species as active sites could significantly improve both the low-temperature and high-temperature catalytic reduction activity of NO_x, especially, its performance maintained unchanged after coating on honeycomb ceramics. Thanks to strong surface acidity sites and the confinement effect, the Cu@ZSM-5 exhibited super activity, high N₂ selectivity, wide operating temperature window and strong water resistance.

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介孔沸石 ZSM-5 内含铜纳米团簇，可高效选择性催化还原 NH3 中的氮氧化物

铜基催化剂因其出色的低温脱硝性能而被广泛应用于氮氧化物的氨选择性催化还原（NH3-SCR）。然而，Cu 物种的聚集一直是催化剂设计中的一个棘手问题。本文通过原位自组装工艺成功构建了球形沸石 ZSM-5 内含铜纳米团簇 Cu@ZSM-5。与 Cu/ZSM-5 相比，它具有高比表面积（373 m2g-1）、更高的 Cu+浓度、丰富的氧空位和更多的酸性位点。结果表明，载体的强酸性位点可提高高温催化活性，而作为活性位点的 Cu 物种可显著提高氮氧化物的低温和高温催化还原活性，特别是在蜂窝陶瓷上涂层后，其性能保持不变。得益于强表面酸性位点和约束效应，Cu@ZSM-5 表现出超强活性、高 N2 选择性、宽工作温度窗口和强耐水性。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.