Precise Control of Aluminum Distribution in Zeolites: Strategies, Characterization, and Perspectives

doi:10.6023/A25100345

Acta Chimica Sinica ›› 2026, Vol. 84 ›› Issue (1): 173-188.DOI: 10.6023/A25100345 Previous Articles

Review

沸石铝分布精准调控: 策略、表征与展望

高红霞^a, 陈慧慧^b, 李林梅^a^,^*(), 赵侦超^a, 徐舒涛^b^,^*()

^a 浙江师范大学化学与材料科学学院先进催化材料教育部重点实验室浙江金华 321004
^b 中国科学院大连化学物理研究所低碳催化与工程研究中心辽宁大连 116023

投稿日期:2025-10-18 发布日期:2025-11-06

作者简介:

高红霞, 浙江师范大学化学与材料科学学院2022级硕士研究生. 主要研究方向为沸石结构单元调控碱处理制备多级孔沸石作用机制.

陈慧慧, 中国科学院大连化学物理研究所博士研究生. 主要研究方向为原位固体核磁研究分子筛酸性质子的离域性质.

李林梅, 浙江师范大学化学与材科学学院, 讲师. 2013年博士毕业于武汉大学分析化学专业. 主要研究方向为基于微流控芯片的电化学分析、材料合成及催化应用.

赵侦超, 浙江师范大学化学与材科学学院, 双龙学者特聘教授. 2007年本科毕业于郑州大学化学系, 2013年博士毕业于中国科学院大连化学物理研究所. 主要研究方向为沸石、氧化铝等催化材料的固体核磁共振表征以及多相催化反应机理研究.

徐舒涛, 中国科学院大连化学物理研究所研究员. 2004年本科毕业于复旦大学化学系, 2010年博士毕业于中国科学院大连化学物理研究所. 现为大连化物所低碳催化技术国家工程研究中心科研骨干. 2016年获第16届国际催化大会青年科学家奖(Young Scientist Prize), 2020年获国家自然科学基金委优秀青年基金资助, 2023年获中国化学会分子筛青年奖. 主要研究方向为原位固体核磁谱学技术在分子筛催化中的应用.

基金资助:
国家自然科学基金(22472153); 国家自然科学基金(22241801); 国家自然科学基金(22032005); 国家自然科学基金(22022202); 浙江省教育厅一般科研项目(Y202456744); 大连市杰出青年科学家基金(2021RJ01); 辽宁国际联合实验室项目(2024JH2/102100005)

Precise Control of Aluminum Distribution in Zeolites: Strategies, Characterization, and Perspectives

Hongxia Gao^a, Huihui Chen^b, Linmei Li^a^,^*(), Zhenchao Zhao^a, Shutao Xu^b^,^*()

^a Key Laboratory of Advanced Catalytic Materials of the Ministry of Education, Zhejiang Normal University, Jinhua, Zhejiang 321004, China
^b National Engineering Research Center of Lower-Carbon Catalysis Technology, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023, China

Received:2025-10-18 Published:2025-11-06
Contact: * E-mail: lilinmei@zjnu.edu.cn;xushutao@dicp.ac.cn
Supported by:
National Natural Science Foundation of China(22472153); National Natural Science Foundation of China(22241801); National Natural Science Foundation of China(22032005); National Natural Science Foundation of China(22022202); Zhejiang Provincial Education Department(Y202456744); Dalian Outstanding Young Scientist Foundation(2021RJ01); Liaoning International Joint Laboratory Project(2024JH2/102100005)

The ultimate goal of heterogeneous catalysis is to precisely regulate chemical reaction transformations. Zeolite catalysts, with their unique shape-selective properties, have been widely used in chemical production, however, achieving highly efficient catalytic reactions requires accurate control over the structure of active sites to minimize side reactions. Since aluminum (Al) atoms located at crystallographically nonequivalent T-sites form the active centers of zeolites, controlling the distribution of Al at both local (T-site level) and spatial (regional) scales has become a research focus in zeolite science. This review systematically summarizes strategies for regulating Al distribution in zeolites—both bottom-up and top-down approaches—as well as advanced characterization techniques. In the bottom-up strategy, using representative zeolite frameworks as examples, we elucidate the mechanism by which organic and inorganic structure-directing agents influence Al distribution. Combined with theoretical calculations, we reveal how van der Waals forces, electrostatic interactions, and hydrogen bonding govern the spatial positioning of Al. In the top-down strategy, selective removal or incorporation of Al atoms is achieved based on variations in the stability of heteroatoms (or Al atoms) at different T-sites, and the advantages and limitations of this method are critically discussed. Accurate characterization of Al distribution is essential for evaluating the effectiveness of regulation strategies; thus, recent advances in Al site characterization are reviewed, emphasizing that multi-technique approaches can yield more reliable structural information. Finally, the review summarizes the merits and drawbacks of each strategy and envisions the future integration of artificial intelligence and big-data-driven high-throughput microchannel zeolite synthesis to realize precise control of Al distribution. The fusion of multiple characterization techniques is further expected to enable accurate structural elucidation, ultimately guiding the rational design of reaction-specific, high-performance zeolite catalysts.

Key words: Al distribution, zeolite, structure directing agent, host-guest interactions, catalysis

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Hongxia Gao, Huihui Chen, Linmei Li, Zhenchao Zhao, Shutao Xu. Precise Control of Aluminum Distribution in Zeolites: Strategies, Characterization, and Perspectives[J]. Acta Chimica Sinica, 2026, 84(1): 173-188.

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Fig. & Tab. 11

Figure 1. Schematic of zeolites with different channel Al distributions and reaction selectivity (a); types of metal ions stabilized by different Al distributions (isolated and paired Al) and active intermediate species (b); and spatial heterogeneity of Al distribution within and on the surface of zeolite crystals (c)

Figure 2. Schematic diagram of FER zeolite structure and distribution of typical OSDAs (a) (Adapted with permission from reference [46], Copyright 2013, American Chemical Society), different OSDAs used to synthesize FER zeolite and the corresponding proportion of acid sites on 8-membered ring cave annotated in parentheses (b), and schematic diagram of interactions between organic/inorganic SDAs and the framework of zeolite (c). * Data adapted from references [47-48]

Figure 3. Schematic draws of common SDAs used to synthesize ZSM-5 zeolite for controlling Al distribution, and the different Al distributions directed by rigid quaternary ammonium salts versus flexible, hydrogen-bond-capable organic amine. (Adapted with permission from reference [63], Copyright 2024, American Chemical Society)

Figure 4. Schematic illustration of the cooperative regulation of isolated Al and Al pairs distribution in SSZ-13 zeolite by TMAda+ with Na+and K+. (Reprinted with permission from reference [70], Copyright 2020, American Chemical Society)

Figure 5. Different organic structure-directing agents (a) and their most stable configurations in the AEI cage, along with the relative energies corresponding to different T-site Al distributions (b)[82]

Figure 6. Schematic diagram illustrating (a) the mechanism of Al distribution in CHA zeolite product governed by FAU precursor during the FAU-to-CHA interzeolite conversion (IZC),[96] and (b) the split synthesis strategy used in the FAU-to-CHA IZC process[101]

Figure 7. Schematic diagram of the mechanism by which SiCl4 removes framework Al from the 12-membered rings of MOR zeolite and replenishes Al distribution in the 8-membered-ring side pockets[118] (Copyright 2022, Wiley-VCH GmbH)

Figure 8. Proposed scheme of dealumination and extraction of EFAl species in small-pore zeolites with 8 membered-ring aperture[126] (Reproduced from Tatsushi Yoshioka et al., Science Advances, doi:10.1126/sciadv.abo3093 [2022], AAAS.)

Figure 9. 27Al MQMAS NMR distinguishing the 27Al NMR signals of different T-site Al in ZSM-5 zeolite (a), and comparison of the experimentally observed 27Al NMR chemical shifts with the distribution of 27Al NMR chemical shifts calculated from the theoretical distribution of Al among different T sites (b)[127] (Copyright 2007, Wiley-VCH GmbH)

Figure 10. 27Al MAS NMR spectra (a, b) and 1H-27Al D-RINEPT spectra (c, d) of MCM-49 (HMI) and MCM-49 (CHA) synthesized using HMI and CHA as structure-directing agents. (Adapted with permission from reference [135], Copyright 2021, American Chemical Society)

Figure 11. Soft X-ray scattering intensity changes of different ZSM-5 zeolite crystal facets under varying energy conditions (resonant, non-resonant) (a); Al atom site occupancies at different T-sites obtained by refinement of scattering signals (b); neutron scattering-derived adsorption configuration of ND3 on ZSM-5 zeolite Brønsted acid sites (c); and NH3 adsorbed on different acid sites and their distances to 27Al nuclei obtained using 15N MAS NMR (d) and 15N-27Al S-RESPDOR (e~f). (Reproduced from Guangchao Li et al., Science, doi:10.1126/science.adq6644 [2025], AAAS.)

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沸石铝分布精准调控: 策略、表征与展望

Precise Control of Aluminum Distribution in Zeolites: Strategies, Characterization, and Perspectives

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