多级孔<strong>ZSM-22</strong>分子筛的合成及其正十二烷加氢异构化性能

doi:10.11901/1005.3093.2025.096

材料研究学报

2026, Vol. 40

Issue (1): 1-12 DOI: 10.11901/1005.3093.2025.096

研究论文

本期目录 | 过刊浏览

多级孔ZSM-22分子筛的合成及其正十二烷加氢异构化性能

韩扬¹^,², 李梦晨³^,⁴, 于宏悦³, 乔亮³, 沈雨歌³, 高善彬³, 矫义来²(

), 迟克彬³(

)

^1.中国科学技术大学材料科学与工程学院沈阳 110016
^2.中国科学院金属研究所沈阳材料科学国家研究中心沈阳 110016
^3.中国石油天然气股份有限公司石油化工研究院北京 102206
^4.清华大学化工系北京 100084

Synthesis of Hierarchical ZSM-22 Zeolite and its Catalytic Performance for Hydrogenation Isomerization of n-Dodecane

HAN Yang¹^,², LI Mengchen³^,⁴, YU Hongyue³, QIAO Liang³, SHEN Yuge³, GAO Shanbin³, JIAO Yilai²(

), CHI Kebin³(

)

^1.School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China
^2.Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
^3.Petrochemical Research Institute, PetroChina Company Limited, Beijing 102206, China
^4.Department of Chemical Engineering, Tsinghua University, Beijing 100084, China

引用本文:

韩扬, 李梦晨, 于宏悦, 乔亮, 沈雨歌, 高善彬, 矫义来, 迟克彬. 多级孔ZSM-22分子筛的合成及其正十二烷加氢异构化性能[J]. 材料研究学报, 2026, 40(1): 1-12.
Yang HAN, Mengchen LI, Hongyue YU, Liang QIAO, Yuge SHEN, Shanbin GAO, Yilai JIAO, Kebin CHI. Synthesis of Hierarchical ZSM-22 Zeolite and its Catalytic Performance for Hydrogenation Isomerization of n-Dodecane[J]. Chinese Journal of Materials Research, 2026, 40(1): 1-12.

全文: PDF(13958 KB) HTML

摘要:

使用十四烷基膦酸(TDPA)介孔模板剂，用水热合成法制备出不同晶粒长度的多级孔ZSM-22分子筛，使用XRD、XRF、SEM、TEM、NH₃-TPD、N₂吸附/脱附、固体NMR以及Py-IR等手段对其表征，研究了正十二烷加氢异构化性能。结果表明，添加TDPA能构筑分子筛的介孔结构并优化酸性分布。在5L规模稳定合成出多级孔ZSM-22，使用这种多级孔分子筛制备出贵金属双功能催化剂并考察其正十二烷的加氢异构化反应性能。结果表明，nTDPA/SiO₂ = 0.0170时合成的ZSM-22分子筛实现了酸性性能和孔结构，使其平均晶粒长度减小至200 nm并具有适宜的酸强度和酸量分布。正十二烷转化率达到83%时异构选择性提高到68%，与常规ZSM-22催化剂(58%)相比提高了10个百分点。

关键词 ：无机非金属材料, 分子筛, 加氢异构化, 介孔, 孔道结构, 酸性, ZSM-22

Abstract：

The zeolite ZSM-22 with different grain length and pore structure was synthesized by hydrothermal synthesis with TDPA as mesoporous template agent. The synthesized material was characterized using XRD, XRF, SEM, TEM, NH₃-TPD, N₂ adsorption/desorption, solid-state NMR, and Py-IR. The results indicated that the incorporation of TDPA is beneficial for the formation of the mesoporous structure and the optimization of the acidity distribution for the prepared ZSM-22 zeolite. Then, a novel bifunctional noble metal catalyst was prepared with the acquired hierarchical ZSM-22 zeolite as support, meanwhile the performance of catalyst in the hydrogenation isomerization of n-dodecane was evaluated. The results revealed that with a molar ratio of nTDPA/SiO₂ of 0.0170, the synthesized ZSM-22 zeolite presented proper pore structure and acidic performance, with an average crystal grain length lowered to 200 nm and an optimal distribution of acid strength and acid sites. For the n-dodecane conversion rate of 83%, the isomer selectivity increased to 68%, representing a 10-percentage-point improvement compared to the conventional blank ZSM-22 catalyst (58%). This study provides a new approach for developing highly efficient hydroisomerization catalyst through the in-situ synthesis of ZSM-22 zeolites with mesoporous structures.

Key words： inorganic non-metallic materials molecular sieves hydroisomerization mesoporous porous structure acidity ZSM-22

收稿日期: 2025-03-04

ZTFLH:

TE65

基金资助:国家重点研发计划(2023YFB3810600);国家自然科学基金(22378407)

通讯作者: 矫义来，研究员，yljiao@imr.ac.cn，研究方向为催化材料;
迟克彬，正高级工程师，ckb459@petrochina.com.cn，研究方向为催化、分离材料

Corresponding author: JIAO Yilai, Tel: (024)23971936, E-mail: yljiao@imr.ac.cn;
CHI Kebin, Tel: (010)80165536, E-mail: ckb459@petrochina.com.cn

作者简介: 韩扬，女，1998年生，硕士生

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https://www.cjmr.org/CN/10.11901/1005.3093.2025.096 或 https://www.cjmr.org/CN/Y2026/V40/I1/1

图1 评价固定床催化剂的装置

图2 不同TDPA添加量ZSM-22分子筛的XRD谱和相对结晶度

表1 不同TDPA添加量合成产物的BET分析结果

图3 合成产物的孔结构

图4 不同TDPA添加量合成产物的SEM照片和频数分布

图5 产物的TEM照片

图6 不同TDPA添加量合成产物的NMR谱

表2 不同TDPA添加量合成产物的硅铝比和NH3-TPD分析结果

图7 不同TDPA添加量合成产物的酸性

表3 不同TDPA添加量合成产物的Py-IR分析结果

图8 Pt/Z22-0.0170-5L的电镜照片

图9 正十二烷加氢异构化的评价结果

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