过渡金属改性Cu-SSZ-13分子筛脱硝催化剂研究进展

doi:10.16085/j.issn.1000-6613.2022-1524

摘要/Abstract

摘要：

氨选择性催化还原技术（NH₃-SCR）是消除氮氧化物最有效的技术之一，高效稳定的催化剂是NH₃-SCR技术的核心。其中Cu基分子筛催化剂特别是Cu-SSZ-13分子筛催化剂受到了广泛的关注与研究，但仍存在着高温活性不好、氮气选择性不够理想和抗硫性能不足等问题。为了进一步提高Cu-SSZ-13分子筛催化剂的脱硝性能，可采用添加过渡金属的方法来改性Cu-SSZ-13分子筛催化剂。本文对过渡金属改性的Cu-SSZ-13分子筛催化剂的研究进展进行了系统的梳理，重点对Fe改性Cu-SSZ-13分子筛催化剂的几种制备方法进行了归纳，分别对离子交换法、浸渍法和一步水热合成法进行了介绍，对几种常见的不同过渡金属（Fe、Mn、Nb、Co、Ni、Ti、Zn）改性的Cu-SSZ-13分子筛催化剂脱硝性能的差别和原因进行了分析和讨论。最后对过渡金属改性的Cu-SSZ-13分子筛脱硝催化剂的研究重点和发展前景进行了展望，指出过渡金属在Cu-SSZ-13分子筛中的具体存在形式、落位情况、协同作用机制等方面的研究有待进一步深入开展。

关键词: 催化剂, 沸石, 选择催化还原, 过渡金属, 改性

Abstract:

Selective catalytic reduction of ammonia (NH₃-SCR) is recognized as one of the most effective technologies for NO _x elimination, and efficient and stable catalysts are the core of NH₃-SCR technology. Cu-based zeolite catalysts, especially Cu-SSZ-13, have attracted extensive attention and research. However, there are still some problems, such as low high temperature activity, insufficient N₂ selectivity and poor sulfur resistance. In order to further improve the denitrification performance of Cu-SSZ-13 zeolite catalysts, transition metal modification can be applied. In this paper, the research progress of Cu-SSZ-13 zeolite catalyst modified by transition metals is reviewed, and the preparation methods of Fe-modified Cu-SSZ-13 zeolite are summarized. The ion exchange method, impregnation method and one-step hydrothermal synthesis method are introduced respectively. The differences and reasons of denitrification performance of Cu-SSZ-13 zeolite modified by different transition metals (Fe, Mn, Nb, Co, Ni, Ti, Zn) are discussed. Finally, the research emphasis and development prospect of Cu-SSZ-13 zeolite catalysts modified by transition metals are prospected, and it concludes that the form, location and synergistic mechanism of transition metals in Cu-SSZ-13 zeolite need to be further studied.

Key words: catalyst, zeolite, selective catalytic reduction, transition metal, modification

中图分类号:

TQ630

殷成阳, 侯铭, 杨爽, 毛迪, 刘俊言. 过渡金属改性Cu-SSZ-13分子筛脱硝催化剂研究进展[J]. 化工进展, 2023, 42(6): 2963-2974.

YIN Chengyang, HOU Ming, YANG Shuang, MAO Di, LIU Junyan. Research progress in transition metals modified Cu-SSZ-13 zeolite denitration catalysts[J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2963-2974.

图/表 9

参考文献 55

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催化剂名称	制备方法	优点	缺点	铁含量	活性窗口/℃	抗性	NO _x 转化率/%	文献
Cu,Fe/SSZ-13	离子交换法	很好地将Fe物种引入催化剂体系	存在固液分离及洗涤等烦琐步骤	0.51%（质量分数）	225~625	—	>90	[14]
CuFe-SSZ-13				0.357%	150~650	—	>98	[16]
Fe_1.32/Cu-SSZ-13				Fe/Cu为1.32	175~550	—	>85	[17]
Ce_0.017-Fe_0.017/Cu-SSZ-13				0.017mol/L Fe³⁺	200~500	抗水硫	>98	[18]
Fe/Cu-SSZ-13(IE)				5.5%	175~500	—	>90	[19]
Fe-Cu-SSZ-13				0.089%	225~625	抗水	>90	[20]
Fe/Cu-SSZ-13	浸渍法	不需要洗涤，用水量最少	引入的Fe物种的落位和分散难控制	1%	250~500	抗硫	>90	[24]
Fe-Cu/SSZ-13-N-1%	浸渍法	不需要洗涤，用水量最少	引入的Fe物种的落位和分散难控制	1.0%	160~530	抗水	>90	[25]
Fe_0.63/Cu_1.50-SSZ-13	一步法	制备过程相对简单	引入的Cu、Fe比例难于控制	0.63%	160~580	抗硫	>90	[26]
Fe_0.5Cu_4.8-SSZ-13				0.5%	200~550	抗水硫	>90	[27]
FeCu-SSZ-13				Fe/Cu为0.2	200~600	—	>90	[28]

催化剂名称	制备方法	优点	缺点	铁含量	活性窗口/℃	抗性	NO _x 转化率/%	文献
Cu,Fe/SSZ-13	离子交换法	很好地将Fe物种引入催化剂体系	存在固液分离及洗涤等烦琐步骤	0.51%（质量分数）	225~625	—	>90	[14]
CuFe-SSZ-13				0.357%	150~650	—	>98	[16]
Fe_1.32/Cu-SSZ-13				Fe/Cu为1.32	175~550	—	>85	[17]
Ce_0.017-Fe_0.017/Cu-SSZ-13				0.017mol/L Fe³⁺	200~500	抗水硫	>98	[18]
Fe/Cu-SSZ-13(IE)				5.5%	175~500	—	>90	[19]
Fe-Cu-SSZ-13				0.089%	225~625	抗水	>90	[20]
Fe/Cu-SSZ-13	浸渍法	不需要洗涤，用水量最少	引入的Fe物种的落位和分散难控制	1%	250~500	抗硫	>90	[24]
Fe-Cu/SSZ-13-N-1%	浸渍法	不需要洗涤，用水量最少	引入的Fe物种的落位和分散难控制	1.0%	160~530	抗水	>90	[25]
Fe_0.63/Cu_1.50-SSZ-13	一步法	制备过程相对简单	引入的Cu、Fe比例难于控制	0.63%	160~580	抗硫	>90	[26]
Fe_0.5Cu_4.8-SSZ-13				0.5%	200~550	抗水硫	>90	[27]
FeCu-SSZ-13				Fe/Cu为0.2	200~600	—	>90	[28]

不同过渡金属改性	过渡金属改性的作用	优点
Fe改性Cu-SSZ-13	Fe物种与Cu物种具有协同作用，提高催化剂的氧化还原能力	NH₃-SCR反应的高温活性好，抗硫性能好
Mn改性Cu-SSZ-13	催化剂酸位点数量增加，Mn和Cu之间相互作用提高催化剂的氧化还原能力	NH₃-SCR反应的低温活性好
Nb改性Cu-SSZ-13	Nb的引入增加了Cu活性物种数量，提高催化剂的氧化还原能力，增强催化剂酸位点	拓宽活性温度窗口范围
Co改性Cu-SSZ-13	Co的引入起占位作用，诱导Cu离子位于具有更高低温活性的1Al位，还可阻止SSZ-13脱铝	NH₃-SCR反应的低温活性好，水热稳定性高
Ni改性Cu-SSZ-13	Ni的引入可以抑制氧化铜形成	提高NH₃-SCR反应的高温活性，进一步拓宽反应的活性温度窗口
Ti改性Cu-SSZ-13	Ti的引入可以保护高温水热过程中分子筛的骨架结构	具有优异的水热稳定性
Zn改性Cu-SSZ-13	Zn的引入有利于Cu物种更好的分散，起到稳定骨架的作用，防止Cu物种发生迁移	拓宽了NH₃-SCR反应活性温度窗口，水热稳定性高

不同过渡金属改性	过渡金属改性的作用	优点
Fe改性Cu-SSZ-13	Fe物种与Cu物种具有协同作用，提高催化剂的氧化还原能力	NH₃-SCR反应的高温活性好，抗硫性能好
Mn改性Cu-SSZ-13	催化剂酸位点数量增加，Mn和Cu之间相互作用提高催化剂的氧化还原能力	NH₃-SCR反应的低温活性好
Nb改性Cu-SSZ-13	Nb的引入增加了Cu活性物种数量，提高催化剂的氧化还原能力，增强催化剂酸位点	拓宽活性温度窗口范围
Co改性Cu-SSZ-13	Co的引入起占位作用，诱导Cu离子位于具有更高低温活性的1Al位，还可阻止SSZ-13脱铝	NH₃-SCR反应的低温活性好，水热稳定性高
Ni改性Cu-SSZ-13	Ni的引入可以抑制氧化铜形成	提高NH₃-SCR反应的高温活性，进一步拓宽反应的活性温度窗口
Ti改性Cu-SSZ-13	Ti的引入可以保护高温水热过程中分子筛的骨架结构	具有优异的水热稳定性
Zn改性Cu-SSZ-13	Zn的引入有利于Cu物种更好的分散，起到稳定骨架的作用，防止Cu物种发生迁移	拓宽了NH₃-SCR反应活性温度窗口，水热稳定性高

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