化工进展 ›› 2025, Vol. 44 ›› Issue (6): 3017-3030.DOI: 10.16085/j.issn.1000-6613.2024-1142

• 专栏:化工生态环境前沿交叉新技术 •    

FeCu-ZSM-5分子筛的绿色合成及其NH3-SCR性能

徐景东1,2(), 刘奔3(), 汪雪琴3, 董鹏4, 席志祥1,2, 徐人威1,2, 岳源源3,4()   

  1. 1.中化石油化工研究院(泉州)有限责任公司,福建 泉州 362100
    2.中化泉州石化有限公司,福建 泉州 362103
    3.福州大学化工学院,福建 福州 350106
    4.清源创新实验室,福建 泉州 362801
  • 收稿日期:2024-07-17 修回日期:2024-09-29 出版日期:2025-06-25 发布日期:2025-07-08
  • 通讯作者: 岳源源
  • 作者简介:徐景东(1984—),男,博士,研究方向为炼化催化技术。E-mail:xujingdong01@sinochem.com
    刘奔(1995—),男,博士,研究方向为工业催化。E-mail:1794569717@qq.com
  • 基金资助:
    国家自然科学基金(22322803);国家自然科学基金(22178059);国家自然科学基金(U23A20113);中化泉州能源科技有限责任公司技术开发合作项目(ZHQZKJ-19-F-ZS-0076)

Green synthesis and NH3-SCR performance of FeCu-ZSM-5 zeolite

XU Jingdong1,2(), LIU Ben3(), WANG Xueqin3, DONG Peng4, XI Zhixiang1,2, XU Renwei1,2, YUE Yuanyuan3,4()   

  1. 1.Sinochem Petroleum Chemical Research Institute(Quanzhou) Co. , Ltd. , Quanzhou 362100, Fujian, China
    2.Sinochem Quanzhou Petrochemical Co. , Ltd. , Quanzhou 362103, Fujian, China
    3.College of Chemical Engineering, Fuzhou University, Fuzhou 350106, Fujian, China
    4.Qingyuan Innovation Laboratory, Quanzhou 362801, Fujian, China
  • Received:2024-07-17 Revised:2024-09-29 Online:2025-06-25 Published:2025-07-08
  • Contact: YUE Yuanyuan

摘要:

FeCu-ZSM-5杂双金属分子筛因在NH3选择催化还原(NH3-SCR)反应中表现出互补优势和协同效应而展现出广阔的应用前景,然而,其制备面临着原料和能源消耗高及污染严重的问题。基于此,开展了以天然矿物为原料无模板剂绿色制备等级孔FeCu-ZSM-5分子筛新工艺的合成研究。在合成过程中以天然矿物为全部硅铝铁源,无外加任何有机模板剂,采用晶种导向合成等级孔FeCu-ZSM-5分子筛。系统考察合成过程关键影响因素,进而确定了最佳的合成条件。考察所制得的等级孔FeCu-ZSM-5分子筛的NH3-SCR性能,并结合一系列表征手段探究等级孔FeCu-ZSM-5分子筛的构效关系。结果表明,Cu的加入可以显著提高FeCu-ZSM-5分子筛的低温脱硝活性,从而拓宽其温窗。Cu的引入不影响FeCu-ZSM-5的拓扑结构,但可对Fe和Cu在分子筛中的位置和分布、分子筛的还原性和酸性进行调控。较高占比的骨架Fe和孤立Cu2+、良好的氧化还原能力和适宜的酸性共同促使FeCu2-ZSM-5分子筛呈现最优异的脱硝性能。

关键词: FeCu-ZSM-5分子筛, 等级孔, 绿色合成, NH3选择催化还原, 协同效应

Abstract:

FeCu-ZSM-5 heterobimetallic zeolite exhibits a broad application prospect in the selective catalytic reduction with ammonia (NH3-SCR) due to the advantage complementary and synergistic effect of different metals, however, its preparation faces serious problems of high material and energy consumption as well as environmental pollution. In view of this, a synthetic study was conducted to explore a new green preparation process for hierarchical FeCu-ZSM-5 zeolite using natural minerals as precursors and without templating agents. During the synthesis process, natural minerals served as the sole source of silica, alumina, and iron, with no organic templating agents added, and a crystal seed inducing synthesis approach was employed. The optimal synthesis conditions were determined by systematically investigating the key influencing factors. The NH3-SCR performance of the synthesized hierarchical FeCu-ZSM-5 was examined, and various characterization techniques were used to probe the structure-performance relationship of the hierarchical FeCu-ZSM-5. The results indicate that the incorporation of Cu significantly enhances the low-temperature denitration activity of the FeCu-ZSM-5 zeolite, thereby expanding its temperature window. The introduction of Cu does not alter the topology of FeCu-ZSM-5 but can modulate the location and distribution of Fe and Cu within the zeolite, as well as its reducing and acidic properties. The presence of higher framework Fe, isolated Cu2+ ions, and good redox capacity and suitable acidity collectively contribute to the superior denitration performance of the FeCu2-ZSM-5 zeolite.

Key words: FeCu-ZSM-5 zeolite, hierarchical pores, green synthesis, NH3-SCR, synergistic effect

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