化工进展2024,Vol.43Issue(5) :2661-2672.DOI:10.16085/j.issn.1000-6613.2023-2088

单晶多级孔ZSM-5分子筛酸性质对正庚烷催化裂解反应传质性能的影响

Effect of acidic properties of single-crystalline hierarchical ZSM-5 zeolite on its activity and mass transfer in n-heptane catalytic cracking

谢小金 张晓雪 刘晓玲 崇明本 程党国 陈丰秋
化工进展2024,Vol.43Issue(5) :2661-2672.DOI:10.16085/j.issn.1000-6613.2023-2088

单晶多级孔ZSM-5分子筛酸性质对正庚烷催化裂解反应传质性能的影响

Effect of acidic properties of single-crystalline hierarchical ZSM-5 zeolite on its activity and mass transfer in n-heptane catalytic cracking

谢小金 1张晓雪 1刘晓玲 2崇明本 2程党国 3陈丰秋3
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作者信息

  • 1. 浙江大学化学工程与生物工程学院,浙江 杭州 310027
  • 2. 浙江大学衢州研究院,浙江 衢州 324000
  • 3. 浙江大学化学工程与生物工程学院,浙江 杭州 310027;浙江大学衢州研究院,浙江 衢州 324000
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摘要

采用L-赖氨酸作为介孔模板剂,通过调控铝源(偏铝酸钠)添加量改变分子筛硅铝比,在单晶分子筛内部引入晶内介孔,成功地合成了一系列具有不同硅铝比的单晶多级孔ZSM-5分子筛,研究了其酸性质对正庚烷催化裂解反应传质性能的影响.利用X射线衍射(XRD)、N2物理吸附、氨气程序升温脱附(NH3-TPD)、吡啶红外(Py-IR)、扫描电子显微镜(SEM)和透射电子显微镜(TEM)等表征了单晶多级孔ZSM-5分子筛的物理结构、酸性质和微观形貌.同时,利用零长柱(ZLC)装置测试获取了正庚烷在单晶多级孔ZSM-5分子筛中的表观扩散系数,用于反映其传质性能.研究结果表明,随着硅铝比的提高,单晶多级孔ZSM-5分子筛的物理结构基本保持一致;传质性能随酸量的减少而提升,催化裂解性能随酸量的增加而提高.当单晶多级孔ZSM-5分子筛的Si/Al从80提高至140,正庚烷的表观扩散系数提升了87%以上;当单晶多级孔ZSM-5分子筛的Si/Al=80时,正庚烷的转化率最高可达97.5%,乙烯和丙烯的选择性分别为24.3%和35.1%.

Abstract

Single-crystalline hierarchical ZSM-5 zeolite with intracrystalline mesopore was successfully synthesized by using L-lysine as a mesoporous template,and the Si/Al ratio was changed by adjusting the adding amount of aluminum source(sodium metaaluminate).Then the effect of acidic properties on zeolite's activity and mass transfer in n-heptane catalytic cracking was investigated in detail.The physical structure,acidic properties and micromorphology of single-crystalline hierarchical ZSM-5 zeolite were characterized by using X-ray diffraction(XRD),nitrogen physical adsorption,ammonia temperature-programmed desorption(NH3-TPD),pyridine infrared(Py-IR),scanning electron microscopy(SEM)and transmission electron microscopy(TEM).In addition,the zero-length column(ZLC)device was employed to test the apparent diffusivity of n-heptane in single-crystalline hierarchical ZSM-5 zeolite,which was used to characterize its mass transfer performance.The results showed that the physical structure of single-crystalline hierarchical ZSM-5 zeolite kept almost the same with the increase of Si/Al ratio,while the zeolite's mass transfer performance was improved with the decrease of acid amount,but the catalytic cracking performance was enhanced with the increase of acid amount.When the Si/Al ratio of the single-crystalline hierarchical ZSM-5 zeolite increased from 80 to 140,the apparent diffusivity of n-heptane could be improved by more than 87%.When the Si/Al ratio was 80,the conversion rate of n-heptane could reach up to 97.5%,and the selectivity of ethylene and propylene were 24.3%and 35.1%,respectively.

关键词

L-赖氨酸/硅铝比/单晶多级孔ZSM-5分子筛/传质/催化/反应

Key words

L-lysine/Si/Al ratio/single-crystalline hierarchical ZSM-5 zeolite/mass transfer/catalysis/reaction

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基金项目

国家自然科学基金(22278353)

出版年

2024
化工进展
中国化工学会,化学工业出版社

化工进展

CSTPCD北大核心
影响因子:1.062
ISSN:1000-6613
参考文献量6
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