ZSM-23沸石纳米片的合成探究

doi:10.1016/S1872-2067(26)65085-1

催化学报 ›› 2026, Vol. 88: 506-515.DOI: 10.1016/S1872-2067(26)65085-1

ZSM-23沸石纳米片的合成探究

刘培^a^,¹, 刘晓娜^b^,¹, 张磊^c, 翟羿^a, 童颜^d, 骆剑锋^a, 吴勤明^a^,^e^,^*(), 陈伟^f^,^*(), 杜晓辉^g, 刘小龙^d, 刘中民^b^,^*(), 肖丰收^a^,^e^,^*()

^a 浙江大学化学工程与生物工程学院, 浙江杭州 310028, 中国
^b 中国科学院大连化学物理研究所, 国家低碳催化技术工程研究中心, 辽宁大连 116023, 中国
^c 常州大学石油化工学院, 先进催化与绿色制造协同创新中心, 江苏省先进催化材料与技术重点实验室, 江苏常州 213164, 中国
^d 中山大学材料学院, 广东广州 510275, 中国
^e 怀柔实验室山西研究院, 山西太原030032, 中国
^f 根特大学分子模拟中心, 东弗兰德省, 比利时
^g 中国石油天然气股份有限公司石油化工研究院兰州化工研究中心, 甘肃兰州 730060, 中国

收稿日期:2025-12-08 接受日期:2026-01-31 出版日期:2026-09-18 发布日期:2026-09-05
通讯作者: *电子信箱: qinmingwu@zju.edu.cn (吴勤明),
Wei.Chen@UGent.be (陈伟),
zml@dicp.ac.cn (刘中民),
fsxiao@zju.edu.cn (肖丰收).
基金资助:
国家重点研发计划(2022YFA1503602);国家自然科学基金(22522208);国家自然科学基金(22288101);国家自然科学基金(22402176);浙江省自然科学基金(LR24B030001);中央高校基本科研业务费专项资金(226-2025-00116);中国石油科技重点研究项目(2023ZZ36)

Insights into synthesis of ZSM-23 zeolite nanosheets

Pei Liu^a^,¹, Xiaona Liu^b^,¹, Lei Zhang^c, Yi Zhai^a, Yan Tong^d, Jianfeng Luo^a, Qinming Wu^a^,^e^,^*(), Wei Chen^f^,^*(), Xiaohui Du^g, Xiaolong Liu^d, Zhongmin Liu^b^,^*(), Feng-Shou Xiao^a^,^e^,^*()

^a College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310028, Zhejiang, China
^b National Engineering Research Center of Lower-Carbon Catalysis Technology, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
^c Collaborative Innovation Center of Advanced Catalysis and Green Manufacturing, Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, Jiangsu, China
^d School of Materials, Sun Yat-Sen University, Guangzhou 510275, Guangdong, China
^e Shanxi Research Institute, Huairou Research Laboratory, Taiyuan 030032, Shanxi, China
^f Center for Molecular Modeling, Ghent University, Technologiepark 46, 9052 Zwijnaarde, Belgium
^g Lanzhou Petrochemical Research Center, Petrochemical Research Institute, PetroChina, Lanzhou 730060, Gansu, China

Received:2025-12-08 Accepted:2026-01-31 Online:2026-09-18 Published:2026-09-05
About author:First author contact:1 共同第一作者.
1 Contributed to this work equally.
Supported by:
National Key Research and Development Program of China(2022YFA1503602);The National Natural Science Foundation of China(22522208);The National Natural Science Foundation of China(22288101);The National Natural Science Foundation of China(22402176);The Zhejiang Provincial Natural Science Foundation of China(LR24B030001);The Fundamental Research Funds for the Central Universities(226-2025-00116);The PetroChina Science and Technology Major Program(2023ZZ36)

摘要/Abstract

摘要：

一维沸石分子筛(如ZSM-23)通常呈现微米级长度的针状形貌, 这种形貌不仅会显著影响催化性能, 也存在潜在的职业健康风险. 本文首次报道了利用一种新型Gemini型季铵盐(Bis-Benz-Pyr²⁺)作为有机模板, 成功合成了厚度仅约10 nm的ZSM-23沸石纳米片; 该模板剂不仅能够导向ZSM-23沸石微孔结构的形成, 并促进纳米片沿a轴和b轴方向生长. 表征结果表明, 所制备的ZSM-23沸石纳米片具有高结晶度、典型的纳米片形貌、较大的外表面积以及完全四配位骨架铝物种. 更重要的是, 在正十六烷加氢异构反应中, 相较于以N,N-二甲基甲酰胺为模板合成的常规ZSM-23沸石, ZSM-23沸石纳米片展现出更高的正十六烷转化率和异十六烷产率. 这些研究结果为后续开发高效沸石催化剂奠定了坚实基础.
X-射线衍射结果证实, 该纳米片具有较高结晶度. 高倍透射电镜结果显示, 沿[001]方向观察, ZSM-23晶体优先沿ab平面生长; 沿[210]方向观察, 其沿[001]方向的厚度约为10 nm. 进一步对纳米片尺寸进行统计分析, 显示其沿a轴、b轴和c轴的尺寸分别为500, 250, 和9 nm. ²⁷Al核磁证实铝物种均为骨架铝; ¹³C核磁表明多数模板剂完整存在于ZSM-23沸石结构中. Ar与N₂吸附结果表明, ZSM-23沸石纳米片具有较大外比表面积; Ar吸附孔径分布图显示其存在32‒80 nm的孔径. 理论模拟表明, Bis-Benz-Pyr²⁺的稳定化能为‒8.73 kJ/(mol·Si), 远低于吡咯烷的‒1.05 kJ/(mol·Si), 证实其是ZSM-23沸石的优良模板剂. 晶面形成能分析显示: 当引入Bis-Benz-Pyr²⁺后, [001]晶面形成能较[010]和[100]更负, 说明沿a, b轴形成纳米片形貌具有热力学优势, 进一步证实该模板剂对ZSM-23沸石纳米片形貌的形成具有关键导向作用. 晶化过程跟踪显示, 随晶化时间延长, ZSM-23沸石纳米片仅沿ab平面扩展, 厚度基本不变, 这一生长特性与理论计算高度一致. 将该纳米片用于正十六烷加氢异构反应, 相较于常规棒状ZSM-23沸石, 其展现出更高的正十六烷转化率和异十六烷收率.
综上, 新型模板剂实现了ZSM-23沸石纳米片的精准合成, 其独特形貌赋予优异催化性能, 为高效沸石催化剂设计提供新思路.

关键词: ZSM-23沸石分子筛, 纳米片, 有机模板, 加氢异构

Abstract:

Precise control of crystal growth allows for zeolites with tailored morphology, and one of the typical zeolite families is one-dimensional zeolites such as ZSM-23, which normally displays a needle-like morphology with micron-level length. This morphology not only strongly influences catalytic performances but also has potentially healthy issue. Herein, we for the first time show a successful synthesis of ZSM-23 zeolite nanosheets with a thickness of only about 10 nm from a novel gemini-type quaternary ammonium as an organic template. Characterizations of the samples demonstrate that ZSM-23 zeolite nanosheets along a and b axes have high crystallinity, large external surface area, and fully four-coordinated aluminum species. Very importantly, ZSM-23 zeolite nanosheets exhibit higher n-hexadecane (C₁₆) conversion and iso-C₁₆ yield in n-C₁₆ hydroisomerization than those of conventional ZSM-23 zeolite synthesized from N,N-dimethylformamide. These findings offer a favorable opportunity for the subsequent development of efficient zeolite catalysts in the future.

Key words: ZSM-23 zeolite, Nanosheets, Organic template, Hydroisomerization

刘培, 刘晓娜, 张磊, 翟羿, 童颜, 骆剑锋, 吴勤明, 陈伟, 杜晓辉, 刘小龙, 刘中民, 肖丰收. ZSM-23沸石纳米片的合成探究[J]. 催化学报, 2026, 88: 506-515.

Pei Liu, Xiaona Liu, Lei Zhang, Yi Zhai, Yan Tong, Jianfeng Luo, Qinming Wu, Wei Chen, Xiaohui Du, Xiaolong Liu, Zhongmin Liu, Feng-Shou Xiao. Insights into synthesis of ZSM-23 zeolite nanosheets[J]. Chinese Journal of Catalysis, 2026, 88: 506-515.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65085-1

https://www.cjcatal.com/CN/Y2026/V88/I9/506

图/表 6

Fig. 1. Low-magnification (A), and high-magnification (B) SEM images, low-magnification TEM image (C), high-magnification TEM images of the ZSM-23-N zeolite nanosheets and the corresponding projections of MTT framework along [001] (D), and [210] (E), respectively. Statistical distribution of nanosheet width (F), length (G), and thickness (H), respectively.

Fig. 2. Characterizations of ZSM-23-N zeolite nanosheets. 27Al MAS NMR (A), 29Si MAS NMR (B), 13C MAS NMR (C) of the template solution (a) and the as-synthesized ZSM-23-N zeolite nanosheets (b) dissolved in HF solution, TG-DTA curves (D), Ar sorption isotherms (E), and pore size distribution (F).

Fig. 3. Structures and stabilization energies of two different OSDAs in ZSM-23 zeolite: Bis-Benz-Pyr2+ (A) and pyrrolidine (B). Zeolite slabs with or without Bis-Benz-Pyr2+ on the surface and the corresponding formation energies: [001] (C), [010] (E), and [100] (G) slabs without OSDA, [001] (D), [010] (F), and [100] (H) slabs with OSDA.

Fig. 4. Crystallization of ZSM-23-N zeolite nanosheets. XRD patterns (A) and SEM images (B) of samples crystallized at 24 h (a), 48 h (b), 60 h (c), 66 h (d), 72 h (e), 78 h (f), 84 h (g), and 90 h (h), respectively. Scale bar = 2 μm.

Fig. 5. High-magnification TEM images of ZSM-23-N zeolite nanosheets crystallized at 24 h (A), 48 h (B), 72 h (C), and 84 h (D).

Fig. 6. Dependences of the n-C16 conversion (A), iso-C16 selectivity (B), and iso-C16 yield (C) as a function of reaction temperature over Pt/H-ZSM-23-N and Pt/H-ZSM-23-C catalysts.

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ZSM-23沸石纳米片的合成探究

Insights into synthesis of ZSM-23 zeolite nanosheets

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