铜基分子筛NH3-SCR催化剂的基本见解:二十年的进展和未来展望

doi:10.1016/S1872-2067(26)65136-4

催化学报 ›› 2026, Vol. 89: 76-101.DOI: 10.1016/S1872-2067(26)65136-4

铜基分子筛NH₃-SCR催化剂的基本见解:二十年的进展和未来展望

刘瑞源^a, 殷成阳^b, 钟城明^a^,^*(), 侯嘉^a, 宋潇飞^a, 刘坚^a, 赵震^a^,^b^,^*()

^a中国石油大学(北京)理学院,重质油国家重点实验室,北京 102249
^b沈阳师范大学化学化工学院,能源与环境催化研究所,辽宁沈阳 110034

收稿日期:2025-12-28 接受日期:2026-02-14 出版日期:2026-10-18 发布日期:2026-09-01
通讯作者: *电子信箱: zhongchengming2022@126.com (钟城明),
zhenzhao@cup.edu.cn/zhaozhen1586@163.com (赵震).
基金资助:
国家自然科学基金(U25A20557);国家自然科学基金(22572131);国家重点研发计划(2021YFB3500601);国家重点研发计划(2021YFB3500603);国家重点研发计划(2022YFB3504100)

Fundamental insight into copper-based zeolite catalysts for NH₃-SCR: Two decades’ progress and future perspectives

Ruiyuan Liu^a, Chengyang Yin^b, Chengming Zhong^a^,^*(), Jia Hou^a, Xiaofei Song^a, Jian Liu^a, Zhen Zhao^a^,^b^,^*()

^aState Key Laboratory of Heavy Oil Processing, China University of Petroleum (Beijing), Beijing 102249, China
^bInstitute of Catalysis for Energy and Environment, College of Chemistry and Chemical Engineering, Shenyang Normal University, Shenyang 110034, Liaoning, China

Received:2025-12-28 Accepted:2026-02-14 Online:2026-10-18 Published:2026-09-01
Contact: *E-mail:zhongchengming2022@126.com(C. Zhong),zhenzhao@cup.edu.cn/zhaozhen1586@163.com(Z. Zhao).
About author:Chengming Zhong (College of Science & State Key Laboratory of Heavy Oil Processing, China University of Petroleum-Beijing) He received his M.S. degree from China University of Petroleum-Beijing in 2020. Since 2020, he has been pursuing his Ph.D. degree at China University of Petroleum-Beijing. His research interests are focused on catalyst design and catalysis nature study for environmental catalysis, especially for vehicle exhaust emission control and industrial flue gas emission control from non-electric industries. He has published 2 peer-reviewed papers and been granted 1 authorized invention patent.
Zhen Zhao (College of Chemistry and Chemical Engineering, Shenyang Normal University) received his Ph.D. degree in 1996 from Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. From 1997 to 2002, he conducted postdoctoral research at National Institute for Resources and Environment (AIST, Japan), National Institute of Industrial Technology (Osaka, Japan), and Lehigh University (USA). Now, he is a Distinguished Professor “Changjiang Scholars Program”, Second Class Professor and Doctoral Supervisor at China University of Petroleum (Beijing); Shenyang Normal University Special Professor Hired, Dean of the College of Chemistry and Chemical Engineering at Shenyang Normal University, and Director of Institute of Catalysis for Energy and Environment. His research interests are focused on catalyst design and catalysis nature study for the energy catalysis; environmental catalysis and rare earth catalysis, especially for diesel exhaust purification, petrochemical conversion of oil and gas, and CO₂ conversion and utilization. He has published more than 600 peer-reviewed papers with over 26800 citations and an H-index of 85, and has been an Elsevier Highly Cited Chinese Researcher for 11 consecutive years with more than 60 authorized invention patents.
Supported by:
National Natural Science Foundation of China(U25A20557);National Natural Science Foundation of China(22572131);National Key R&D Program of China(2021YFB3500601);National Key R&D Program of China(2021YFB3500603);National Key R&D Program of China(2022YFB3504100)

摘要/Abstract

摘要：

氨选择性催化还原(NH₃-SCR)技术凭借其高效、成熟的工艺优势, 依然是当前脱除NO_x的主流后处理方案. 在众多催化剂体系中, 铜交换分子筛(Cu基分子筛)因其优异的宽温窗口及环境友好特性, 被公认为该领域的代表性催化剂. 然而, 实际工况中复杂的水热老化、硫中毒等问题严重制约了催化剂的长周期稳定运行. 深入理解其构效关系与失活机制对于推动下一代高性能催化剂的理性设计具有重要理论价值与实践意义. 基于此, 本文系统梳理了Cu基分子筛的研究进展, 旨在建立从基础认知到实际应用的完整知识体系.

本文遵循“结构-性能-机理-优化”的逻辑主线, 首先评述了MFI, CHA, AEI, LTA等典型分子筛拓扑结构的催化特性, 从微观角度揭示了孔道结构、酸性位分布对NO_x转化效率的调控规律. 在反应机理层面, 本文整合了双ZCuOH活性位点上连续双NO活化的完整反应路径, 进一步完善了经典的L-NH₃(NH₃结合于溶剂化Cu²⁺离子)还原半环活化模型, 为理解Cu基分子筛的本征催化活性提供了更为精确的理论框架. 针对水热稳定性这一关键瓶颈, 本文深入总结了Cu-SSZ-13分子筛水热老化的基本原理与最新研究见解, 并着重论证了Cu-SSZ-39作为新一代优选候选材料的结构优势. 在抗中毒性能方面, 本文细致剖析了Cu-CHA催化剂的SO₂中毒微观机制, 提出通过原子尺度精准调控Cu物种的分布状态, 可实现抗硫性能与水热稳定性的协同提升. 此外, 本文还系统评估了构建保护/牺牲位点、共结晶策略及核壳结构设计等补充改性手段的积极作用. 面对未来扩散限制带来的传质挑战, 本文特别关注了二维PST-9分子筛与OFF/ERI共生分子筛等新型材料体系的开发潜力, 为突破传统三维分子筛的孔道限制提供了新思路.

展望未来, Cu基分子筛催化剂将持续朝着更高活性、更强耐久性、更低成本的方向演进. 随着合成化学、表征技术与计算模拟的深度融合, 数据驱动的催化剂高通量筛选与智能设计将逐步落地. 本文建立的结构-性能关联规律与失活机制解析方法, 将为领域创新发展提供坚实支撑, 最终推动NH₃-SCR技术在严苛排放法规下实现工程化应用与产业化升级.

关键词: 铜基分子筛, 氨选择性催化还原, 反应机理, 水热稳定性, 抗硫性

Abstract:

Amidst tightening mobile-source emission regulations, ammonia selective catalytic reduction remains the dominant post-treatment technology for NO_x removal, with copper-exchanged zeolites (Cu-zeolites) serving as benchmark catalysts. Here, we systematically survey zeolite topologies—such as MFI, CHA, AEI, and LTA—evaluating their catalytic performance, reaction mechanisms, hydrothermal stability, and resistance to poisoning. A comprehensive overall pathway of sequential two-NO activation on dual ZCuOH sites is unified and complements the established L-NH₃ (NH₃ bond to solvated Cu²⁺ ions) activation model in the Reduction Half-Cycle. This work provides fundamental insights into the performance, hydrothermal stability, and SO₂ resistance of Cu-based zeolites. Therefore, the fundamentals and new mechanistic insights of hydrothermal aging are summarized over Cu-SSZ-13, while highlighting Cu-SSZ-39 as an intrinsically robust successor. We dissect the SO₂ poisoning mechanisms of Cu-CHA, demonstrating that engineering the atomic-scale distribution of Cu enhances both sulfur tolerance and hydrothermal stability. Supplementary strategies (e.g., constructing protective/sacrificial sites, co-crystallization, and core-shell structures) are also considered beneficial. Beyond durability, we also focus on the two-dimensional PST-9 zeolite and OFF/ERI intergrowths zeolite for the future challenge of diffusion. Finally, we outline future research frontiers, aiming to unify Cu-zeolite theory into a mechanistic framework that translates fundamental insights into rational design principles for next-generation catalysts.

Key words: Cu-zeolites, Ammonia selective catalytic reduction, Reaction mechanism, Hydrothermal stability, Sulfur tolerance

刘瑞源, 殷成阳, 钟城明, 侯嘉, 宋潇飞, 刘坚, 赵震. 铜基分子筛NH₃-SCR催化剂的基本见解:二十年的进展和未来展望[J]. 催化学报, 2026, 89: 76-101.

Ruiyuan Liu, Chengyang Yin, Chengming Zhong, Jia Hou, Xiaofei Song, Jian Liu, Zhen Zhao. Fundamental insight into copper-based zeolite catalysts for NH₃-SCR: Two decades’ progress and future perspectives[J]. Chinese Journal of Catalysis, 2026, 89: 76-101.

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图/表 27

Fig. 1. The contents of this paper.

Fig. 2. Low temperature NH3-SCR reaction mechanisms and strategies for diffusion limitation, hydrothermal stability, and SO2 resistance of Cu based zeolite.

Table 1 The range of activity prepared by different methods (ZSM-5).

Catalyst	Active range	Preparation method	Conditions	Ref.
3.5Cu/0.6NaZSM-5	220-400 °C (T₈₀)	Ion exchange method	200 ppm NO, 200 ppm NH₃, 10% O₂, 6% H₂O, GHSV = 125000 h^-1	[52]
Cu-ZSM-5-ZrO₂	210-400 °C (T₈₀)	Ion exchange method	500ppm NO, 500 ppm NH₃, 10% O₂, 1.5% H₂O, GHSV = 28000 h^-1	[53]
CuCe/ZSM-5	250-400 °C (T₉₀)	Impregnation method	1000 ppm NO, 1100 ppm NH₃, 5% O_2，10% H₂O, GHSV = 30000 h^-1	[54]
Ce₁-Cu₄/ZSM-5	185-470 °C (T₉₀)	Impregnation method	500 ppm NO, 500 ppm NH₃, 5% O₂, GHSV = 55000 h^-1	[55]
Cu-Zr/ZSM-5	167-452 °C (T₉₅)	Ion exchange method	1000 ppm NO, 1000 ppm NH₃, 10% O₂, GHSV = 100000 h^-1	[56]
CuCe_0.75Zr_0.25/ZSM-5	175-468 °C (T₉₅)	Ion exchange method	1000 ppm NO, 1000 ppm NH₃, 10% O₂, GHSV = 15000 h^-1	[57]
NS_L-Cu-ZSM-5	250-550 °C (T₁₀₀)	Ion exchange method	1000 ppm NO, 1000 ppm NH₃, 8% O₂, 5% H₂O, GHSV = 50000 h^-1	[73]

Fig. 3. Reaction mechanism of the NH3-SCR reaction over ZCuOH species. (a) Reprinted with permission from Ref. [72]. Copyright 2021, American Chemical Society. (b) Reprinted with permission from Ref. [29]. Copyright 2023, American Chemical Society.

Table 2 The range of activity prepared by different methods (SSZ-13).

Catalyst	Active range	Preparation method	Conditions	Ref.
Cu-SSZ-13	170-450 °C (T₉₀)	one-pot method	1000 ppm NO, 1000 ppm NH₃, and 10% O₂,	[110]
Cu-SSZ-13	245-460 °C (T₉₀)	one-pot method	500 ppm NO, 530 ppm NH₃, 7% O₂, 5% H₂O, GHSV = 450000 h^-1	[111]
Cu-SSZ-13	250-550 °C (T₉₀)	one-pot method	500 ppm NO, 500 ppm NH₃, 5% O₂, GHSV = 800000 h^-1	[112]
Cu&Zn-SSZ-13	200-600 °C (T₉₀)	one-pot method	600 ppm NO, 600 ppm NH₃, 6% O₂, 5 % H₂O, GHSV ≈ 400000 h^-1	[113]
Cu, M/SSZ-13	250-500 °C (T₉₅)	ion exchange method	350 ppm NO, 350 ppm NH₃, 14% O₂, 2.5% H₂O, GHSV = 100000 h^-1	[116]
Cu-Na-SSZ-13	150-650 °C (T₈₅)	ion exchange method	500 ppm NO, 500 ppm NH₃, 10% O₂, 5% H₂O, GHSV = 80000 h^-1	[104]

Fig. 6. The location of Cu and its migration in different atmospheres. (a) Relative binding energy of Cu2+-2Z under different possible Al arrangements. Reprinted with permission from Ref. [133]. Copyright 2021, Elsevier B.V. (b) HSE06-optimized structures of Cu sites. Reprinted with permission from Ref. [130]. Copyright 2016, American Chemical Society. (c) Cu positions (gray balls) visited during 90 ps of NVT AIMD at 298 K. Reprinted with permission from Ref. [130]. Copyright 2016, American Chemical Society. (d) Cu positions (gray balls) sampled inside the zeolite cage during 90 ps of equilibrated NVT AIMD at 473 K for the most stable NH3-solvated CuI and CuII species. Reprinted with permission from Ref. [130]. Copyright 2016, American Chemical Society. (e) Reactant state (1) [CuI(NH3)2 in the same cage as Al], transition state (2) [CuI(NH3)2 diffusion through 8-MR], and product state (3) [CuI(NH3)2 in the neighboring cage without Al]. Reprinted with permission from Ref. [135]. Copyright 2017, The American Association for the Advancement of Science.

Fig. 7. Proposed low-temperature SCR catalytic cycle. (a) Reprinted with permission from Ref. [142]. Copyright 2017, American Chemical Society. (b) Reprinted with permission from Ref. [135]. Copyright 2017, The American Association for the Advancement of Science.

Fig. 9. (a) (I) Phase-uncorrected k2-weighted FT-EXAFS curves during exposure of the Cu-CHA catalyst to NO/NH3/He (dark blue thick line), followed by 10% O2 in He (gray thin lines; red thick line: final spectrum; dark gray dashed line: pretreatment in O2 by heating in O2 up to 400 °C and subsequently cooling in O2 down to 200 °C prior to XAS data collection, step 1. (II) Illustration of [Cu(NH3)2]+ and (III) μ-η2, η2-peroxo diamino dicopper (side-on) complexes. Atom color code: Cu, green; H, white; O, red; N, blue. Reprinted with permission from Ref. [155]. Copyright 2020, American Chemical Society. (b) Simulation of O2 adsorption and oxidation of two CuI(NH3)2 equivalents. Reprinted with permission from Ref. [135]. Copyright 2017, The American Association for the Advancement of Science.

Fig. 10. Ex-situ Cu speciation phase diagrams based on HSE06-Tsvdw calculations on 1Al (a) and 2Al (b) Cu exchange sites. Regions indicate site composition that minimizes free energy at 2% H2O and given T and PO2. Reprinted with permission from Ref. [130]. Copyright 2016, American Chemical Society.

Fig. 11. (a) Schematic illustration of dynamic 15NH3 exchange between NH4+ and [Cu(NH3)2]+ species in Cu-CHA. Framework Si and Al atoms are depicted in blue and red, respectively, while Cu cations are shown in gold, with orange arrows indicating possible exchange pathways within the Cu-CHA pores. (b) Solid-state 2D exchange 15N NMR spectrum of fresh Cu-CHA recorded at 53 °C following 15NH3 exposure at 120 °C and subsequent reduction in 15NO at 300 °C; 1D projections are displayed along the horizontal and vertical axes. (c) Evolution of on-diagonal (red and blue) and off-diagonal (orange) peak intensities as a function of mixing time in 2D 15N exchange NMR spectra acquired at 53 °C, 11.7 T, and 12.5 kHz MAS for fresh Cu-CHA. (d) Eyring plots of temperature-dependent exchange rate coefficients derived from global fitting of data such as those in panel (c), measured at 41, 53, and 66 °C for fresh (black), 4-h-aged (red), and 16-h-aged (blue) Cu-CHA catalysts; error bars represent uncertainties estimated via Monte Carlo error propagation. Reprinted with permission from Ref. [171]. Copyright 2025, American Chemical Society.

Fig. 13. Schematic diagram of the preparation of a core-shell catalyst. (a) Cu-Ce-La/SSZ-13@ZSM-5 core-shell catalyst. Reprinted with permission from Ref. [195]. Copyright 2020, Elsevier B.V. (b) Cu-SSZ-13@CZO core-shell catalyst. Reprinted with permission from Ref. [196]. Copyright 2022, American Chemical Society.

Table 3 The activity range after hydrothermal aging (SSZ-39).

Catalyst	Active range	Conditions	Ref.
Cu-SSZ-39	250-550 °C (T₈₀)	800 °C, 12 h	[243]
MnCu-SSZ-39	250-550 °C (T₉₀)	850 °C, 12 h	[279]
Cu-SSZ-39	225-450 °C (T₉₀)	900 °C, 5 h	[280]
Cu/Y-SSZ-39	200-550 °C (T₇₀)	900 °C, 10 h	[250]
Cu-SSZ-39	225-500 °C (T₈₅)	850 °C, 16 h	[244]
Cu-Y-SSZ-39	200-550 °C (T₈₀)	940 °C, 3 h	[245]

Fig. 17. The supposed reaction mechanism of NH3-SCR on Cu/SSZ-39. (a) Reprinted with permission from Ref. [248]. Copyright 2021, Elsevier B.V. (b) Reprinted with permission from Ref. [249]. Copyright 2021, American Chemical Society.

Fig. 18. Structure of the fresh, dehydrated Cu-LTA-16-0.48 catalyst. A Cu2+ cation located at the center of a single 6-ring is shown at the right. Reprinted with permission from Ref. [33]. Copyright 2017, Wiley-VCH.

Fig. 20. (a) HRTEM image of as-made ChRbLi-PST-9. (b) ADF-STEM image of ChRbLi-PST-9 obtained along the b-axis after sectioning the nanosheet by ultramicrotome. (c) Projected potential map constructed based on the ADF-STEM image in plane group pmg showing the structure of PST-9 viewed along the b-axis. (d) Simulated powder XRD pattern. (e) Simulated 29Si MAS NMR spectra of as-made ChRbLi-PST-9. (f) 1H NMR spectra of organic SDA, choline. (g,h) Structures of PST-9 along the b-axis and c-axis. Reprinted with permission from Ref. [269]. Copyright 2019, Wiley-VCH.

Fig. 22. (a-d) SCR reaction rates at different temperatures of Cu-T, Cu-ERI, and Cu-OFF before and after hydrothermal aging treatment, and in-situ DRIFTS spectra of NO + O2 saturation adsorption. (e) NH4NO3 decomposition pathway assisted with/without BAS. Reprinted with permission from Ref. [276]. Copyright 2024 American Chemical Society.

Fig. 23. (a) OSDA reported to crystallize CHA and ERI with the candidate OSDA presented. (b) Comparison between the templating energies of the OSDAs with the CHA and ERI frameworks. (c) Relationship between the shape of the OSDAs and their binding energies toward CHA or ERI. Reprinted with permission from Ref. [277]. Copyright 2024, American Chemical Society.

Table 4 Comparison of Cu-zeolite catalysts with different topological structures.

Catalyst	Topological structure	Cu location	Active range (fresh)	Active range (aged)	Primary applications
Cu-ZSM-5	MFI	10-MR, 6-MR	200-450 °C	poor	low-temperature stationary sources
Cu-SSZ-13	CHA	6-MR, 8MR	180-550 °C	225-450 °C (T₉₀, 800 °C, 16 h)	diesel vehicle exhaust
Cu-SSZ-39	AEI	6-MR, 8MR	225-550 °C	225-500 °C (T₈₅, 850 °C, 16 h)	next-generation diesel vehicles
Cu-LTA	LTA	6-MR	250-580 °C	225-500 °C (T₉₀, 900 °C, 24 h)	high-temperature stationary sources
Cu-SSZ-16	AFX	gme, aft	175-600 °C	225-450 °C (T₈₅, 800 °C, 16 h)	gas turbine
Cu-PST-9	PST-9	8-MR	220-500 °C	225-500 °C (T₈₀)	multifunctional catalysis
Cu-OFF/ERI	OFF/ERI	interface 6-MR	175-550 °C	225-500 °C (T₉₀, 750 °C, 16 h)	alternative Cu-SSZ-13

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铜基分子筛NH₃-SCR催化剂的基本见解:二十年的进展和未来展望

Fundamental insight into copper-based zeolite catalysts for NH₃-SCR: Two decades’ progress and future perspectives

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