金属负载型分子筛催化剂的NH<sub>3</sub>-SCR机理研究进展

张文博; 陈佳玲; 郭立; 郑伟; 王光华; 郑申棵; 吴晓琴

doi:10.1016/S1872-5813(21)60080-4

金属负载型分子筛催化剂的NH₃-SCR机理研究进展

doi: 10.1016/S1872-5813(21)60080-4

张文博^1,,
陈佳玲^1, ,,
郭立¹,
郑伟¹,
王光华¹,
郑申棵^2, ,,
吴晓琴^1, ,

1.
武汉科技大学化学与化工学院煤转化与新型炭材料湖北省重点实验室，湖北武汉 430081
2.
黄冈师范学院化学化工学院催化材料制备与应用湖北省重点实验室，湖北黄冈 438000

基金项目: 国家自然科学基金（22002114），武汉市科技局项目（2018060401011311）和国家重点研发计划（2017YFB0304303）资助

详细信息

通讯作者:
Tel：027-87643502, E-mail：chenjialing@wust.edu.cn

zhengshenke@163.com

wuxiaoqin@wust.edu.cn

中图分类号: X511
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- 被引次数: 0
出版历程
- 收稿日期: 2021-03-11
- 修回日期: 2021-04-07
- 网络出版日期: 2021-04-19
- 刊出日期: 2021-09-30

Research progress on NH₃-SCR mechanism of metal-supported zeolite catalysts

ZHANG Wen-bo^1
,,
CHEN Jia-ling^{1
, ,},
GUO Li¹,
ZHENG Wei¹,
WANG Guang-hua¹,
ZHENG Shen-ke^{2
, ,},
WU Xiao-qin^{1
, ,}

1.
Key Laboratory of Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, China
2.
Hubei Key Laboratory for Processing and Application of Catalytic Materials, School of Chemistry and Chemical Engineering, Huanggang Normal University, Huanggang 438000, China

Funds: The project was supported by the National Natural Science Foundation of China (22002114), the Wuhan Science and Technology Bureau (2018060401011311) and the National Key Research and Development Program (2017YFB0304303)

摘要

摘要: 在NH₃选择性催化还原（NH₃-SCR）反应中，由于具有宽温度窗口和良好的水热稳定性，金属负载型分子筛是具有广泛应用潜力的脱硝催化剂。本文综述了Cu基和Fe基分子筛催化剂在NH₃-SCR领域的研究进展，总结了催化剂的结构特征和NH₃-SCR性能指标，并对相应的金属活性位点和反应机理进行了归纳。此外，系统介绍了密度泛函理论（DFT）计算在NH₃-SCR反应机理中的应用及反应动力学的研究方法，并对比了不同催化剂体系下的表观动力学参数，为进一步研究金属负载型分子筛催化剂的NH₃-SCR反应机理提供方法与思路。
- NH₃-SCR /
- 分子筛 /
- 反应机理 /
- 反应动力学
Abstract: Metal-supported zeolite catalysts have been widely used in the NH₃ selective catalytic reduction (NH₃-SCR) reactions due to their wide temperature window and good hydrothermal stability. In this review, the research progress in the structural characteristics, catalytic performance and reaction mechanism of Cu- and Fe-based zeolite catalysts in NH₃-SCR was summarized. In addition, the application of density functional theory (DFT) calculation in clarifying the reaction mechanism of NH₃-SCR was introduced. Finally, the reaction kinetics and the apparent kinetic parameters of different metal-based zeolite catalysts in NH₃-SCR were compared and discussed. We hope this review could provide new ideas for the study of NH₃-SCR reaction mechanism over metal-supported zeolite catalysts.
- NH₃-SCR /
- zeolite /
- reaction mechanism /
- reaction kinetics

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FIG. 914. FIG. 914.

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图 1 铁基分子筛中Fe^II与NO的配位研究^[70]

Figure 1 Coordination of Fe^II with NO in Fe-based zeolite^[70]

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图 2 金属负载型分子筛催化剂上NH₃-SCR的反应路径^[3]

Figure 2 NH₃-SCR reaction pathway over metal-based zeolite catalysts^[3]

(with permissions from ACS publications)

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图 3 铁基分子筛在NH₃-SCR反应中可能形成的中间态过渡配合物

Figure 3 Possible intermediate complexes formed on Fe-based zeolites in NH₃-SCR

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图 4 Cu/SSZ-13上硝酸盐与亚硝酸盐类中间体的形成与分解^[37]

Figure 4 Formation and decomposition of nitrate and nitrite intermediates on Cu/SSZ-13^[37]

(with permissions from ACS publications)

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图 5 Cu/SSZ-13的六元环平面上的Cu²⁺化学环境变化^[79]

Figure 5 Changes of the local copper environment in d6r subunit of Cu/SSZ-13^[79]

(with permissions from ACS publications)

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图 6 Cu/SAPO-34上不同反应路径的自由能变化^[116]

Figure 6 Free energy diagrams of different reaction paths on Cu/SAPO-34^[116]

(with permissions from ACS publications)

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表 1 代表性的铁基NH₃-SCR分子筛催化剂

Table 1 Summary of representative Fe-based NH₃-SCR zeolites catalysts

Catalyst	Topology	Channel system	Preparation method	Metal content w/%	Reaction condition	Temperature window/℃	NO_x conversion	Ref.
Fe/ZSM-5	MFI	3-dimensiona l10-MR	IE^a	1.9	0.1% NO，0.1% NH₃，5% O₂，6% H₂O，balance of He，GHSV = 1.9 × 10⁵h⁻¹	300−550	> 80%	[59]
Fe/Beta	BEA	3-dimensiona l12-MR	CVD^b	4.7	0.1% NO，0.12% NH₃，8% O₂，8% H₂O，10%CO₂，balance of N₂，GHSV = 2.1 × 10⁵h⁻¹	300−500	> 90%	[60]
Fe/Mordenite	MOR	1-dimensiona l12-MR	IE	2.3	0.05% NO，0.05% NH₃，5% O₂，balance of N₂，GHSV = 1.6 × 10⁴h⁻¹	350−500	100%	[61]
Fe/SSZ-13	CHA	3-dimensiona l8-MR	IE	1.37	0.035% NO，0.035% NH₃，14% O₂，2.5% H₂O，balance of N₂，GHSV = 2 × 10⁵h⁻¹	320−550	> 80%	[50]
Fe-SAPO-34	CHA	3-dimensiona l8-MR	OP^c	1.0	0.035% NO，0.035% NH₃，14% O₂，5%CO₂，balance of Ar，GHSV = 3.0 × 10⁴h⁻¹	300−600	> 80%	[51]
Fe/Ferrierite	FER	2-dimensiona l10-MR	CVD	4.7	0.1% NO，0.12% NH₃，8% O₂，8% H₂O，10%CO₂，balance of N₂，GHSV = 2.1 × 10⁵h⁻¹	250−500	> 90%	[60]
Fe-SSZ-39	AEI	3-dimensiona l8-MR	OP	1.01	0.005% NO，0.006% NH₃，10% O₂，10% H₂O，balance of N₂，GHSV = 4.5 × 10⁵h⁻¹	300−550	> 90%	[57]
Fe/L	LTL	1-dimensiona l12-MR	CVD	5.1	0.1% NO，0.12% NH₃，8% O₂，8% H₂O，10%CO₂，balance of N₂，GHSV = 2.1 × 10⁵h⁻¹	300−500	> 80%	[60]
Fe-ERI	ERI	3-dimensiona l8-MR	OP	1.03	0.05% NO，0.06% NH₃，10% O₂，10% H₂O，balance of N₂，GHSV = 1 × 10⁵h⁻¹	450−550	> 60%	[62]
Fe-SSZ-16	AFX	3-dimensiona l8-MR	OP	0.95	0.05% NO，0.05% NH₃，5% O₂，10% H₂O，balance of N₂，GHSV = 1 × 10⁵h⁻¹	400−550	> 80%	[62]
Fe-MCM-22	MWW	2-dimensiona l10-MR	OP	4.8	0.05% NO，0.05% NH₃，5% O₂，balance of N₂，GHSV = 6 × 10⁴h⁻¹	190−490	> 80%	[23]
Fe/LTA	LTA	3-dimensiona l8-MR	IE	1.8	0.05% NO，0.05% NH₃，5% O₂，10% H₂O，balance of N₂，GHSV = 1 × 10⁵h⁻¹	370−580	> 90%	[58]
Fe/UZM-35	MSE	3-dimensiona l12-MR	IE	1.9	0.05% NO，0.05% NH₃，5% O₂，10% H₂O，balance of N₂，GHSV = 1 × 10⁵h⁻¹	250−570	> 90%	[56]
^a: ion-exchange; ^b: chemical vapor deposition; ^c: one-pot

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表 2 代表性的铜基NH₃-SCR分子筛催化剂总结

Table 2 Summary of representative Cu-based NH₃-SCR zeolites catalysts

Catalyst	Topology	Channel system	Preparation method	Metal content w/%	Reaction condition	Temperature window/℃	NO_x conversion	Ref.
Cu/ZSM-5	MFI	3-dimensiona l10-MR	IE^a	4.7	0.05% NO，0.05% NH₃，5% O₂， 10%H₂O，balance of N₂，GHSV = 1.0 × 10⁵h⁻¹	150−450	> 80%	[89]
Cu/Beta	BEA	3-dimensiona l12-MR	IE	2.1	0.075% NO，0.075% NH₃，9.5% O₂，balance of Ar，GHSV = 9 × 10⁴h⁻¹	280−520	> 70%	[90]
Cu/SSZ-13	CHA	3-dimensiona l8-MR	IE	3.6	0.05% NO，0.05% NH₃，5% O₂， 10% H₂O，balance of N₂，GHSV = 4.0 × 10⁵h⁻¹	200−550	> 85%	[91]
Cu/SAPO-34	CHA	3-dimensiona l8-MR	IE	1.89	0.05% NO，0.05% NH₃，5% O₂，balance of N₂，GHSV = 6.0 × 10³ h⁻¹	190−540	> 80%	[52]
Cu/SAPO STA-7	SAV	3-dimensiona l8-MR	IE	3.3	0.05% NO，0.05% NH₃，5% O₂，balance of N₂，GHSV = 1 × 10⁵h⁻¹	250−350	> 80%	[84]
Cu/SAPO STA-7	SAV	3-dimensiona l8-MR	DS^b	4.2	0.05% NO，0.05% NH₃，5% O₂，balance of N₂，GHSV = 1 × 10⁵h⁻¹	200−400	> 80%	[84]
Cu/SSZ-16	AFX	3-dimensiona l8-MR	IE	5.65	0.05% NO，0.05% NH₃，10% O₂，balance of N₂，GHSV = 4.25 × 10⁴h⁻¹	200−500	> 90%	[52]
Cu/Nu-3	LEV	2-dimensiona l8-MR	IE	0.79	0.05% NO，0.05% NH₃，10% O₂，balance of N₂，GHSV = 4.25 × 10⁴h⁻¹	270−420	> 90%	[52]
Cu/Sigma-1	DDR	2-dimensiona l8-MR	IE	0.82	0.05% NO，0.05% NH₃，10% O₂，balance of N₂，GHSV = 4.25 × 10⁴h⁻¹	230−450	> 90%	[52]
Cu/SSZ-39	AEI	3-dimensiona l8-MR	IE	0.52	0.05% NO，0.05% NH₃，7% O₂，balance of N₂，GHSV = 2.7 × 10⁵h⁻¹	220−550	> 90%	[92]
Cu/ERI	ERI	3-dimensiona l8-MR	IE	2.2	0.05% NO，0.053% NH₃，7% O₂，5% H₂O，balance of N₂，GHSV = 1 × 10⁵h⁻¹	250−500	> 80%	[62]
Cu/SSZ-16	AFX	3-dimensiona l8-MR	IE	3.0	0.05% NO，0.053% NH₃，7% O₂，5% H₂O，balance of N₂，GHSV = 1 × 10⁵h⁻¹	270−550	> 90%	[62]
Cu/SAPO-18	AEI	3-dimensiona l8-MR	IE	5.6	0.05% NO，0.053% NH₃，7% O₂，5% H₂O，balance of N₂，GHSV = 4.5 × 10⁵h⁻¹	240−460	> 90%	[82]
Cu/KFI	KFI	3-dimensiona l8-MR	IE	4.7	0.05% NO，0.05% NH₃，8% O₂，5% H₂O，balance of N₂，GHSV = 1.2 × 10⁵h⁻¹	250−500	> 90%	[93]
Cu/RHO	RHO	3-dimensiona l8-MR	IE	2.4	0.05% NO，0.05% NH₃，5% O₂， 10% H₂O，balance of N₂，GHSV = 1 × 10⁵h⁻¹	250−500	> 90%	[94]
Cu/SAPO-44	CHA	3-dimensiona l8-MR	IE	1.59	0.05% NO，0.05% NH₃，5.3% O₂，balance of He，GHSV = 1 × 10⁵h⁻¹	180−550	> 90%	[83]
Cu/LTA	LTA	3-dimensiona l8-MR	IE	2.7	0.05% NO，0.05% NH₃，5% O₂， 10% H₂O，balance of N₂，GHSV = 1 × 10⁵h⁻¹	220−600	> 90%	[85]
Cu/UZM-35	MSE	3-dimensiona l12-MR	IE	3.3	0.05% NO，0.05% NH₃，5% O₂， 10% H₂O，balance of N₂，GHSV = 1 × 10⁵h⁻¹	200−550	> 90%	[88]
^a: ion-exchange, ^b: directly synthesised

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表 3 各铁基和铜基分子筛催化剂上标准NH₃-SCR反应的表观反应活化能

Table 3 Apparent activation energy values of standard NH₃-SCR reactions over Fe- and Cu-based zeolite catalysts

Catalyst	Temperature range t/℃	E_a/（kJ·mol⁻¹）	Ref.
Cu/ZSM-5	150−240	42	[120]
Fe/ZSM-5	200−250	46	[121]
Cu/BEA	100−140	58.9	[122]
Fe/BEA	350−400	48	[56]
Cu/MOR	200−250	35	[123]
Fe/MOR	220−320	58	[124]
Cu/SSZ-13	100−200	43	[125]
Fe/SSZ-13	220−270	48	[76]
Cu/SAPO-34	100−200	33.6	[101]
Cu/SAPO-18	150−180	58.3	[126]
Cu/KFI	140−180	53	[93]
Cu/FAU	190−240	29	[127]
Cu/SAPO-44	150−200	38.2	[83]
Cu/LTA	170-200	43	[86]
Fe/LTA	350−400	49	[56]
Fe/UZM-35	350−400	48	[56]

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