| 含骨架铁ZSM-5的合成及其负载Pt催化剂在正十二烷脱氢反应中的催化性能 |
| Synthesis of ZSM-5 Containing Framework Iron and Catalytic Performance of Supported Pt Catalysts in Dehydrogenation of n-Dodecane |
| 作者 | 单位 | E-mail | | 崔孟涛 | 常州大学石油化工学院, 江苏省绿色催化材料与技术重点实验室, 常州 213164
中国科学院青岛生物能源与过程研究所, 生物燃料重点实验室, 青岛 266101 | | | 王忠 | 中国科学院青岛生物能源与过程研究所, 生物燃料重点实验室, 青岛 266101 | | | 李学兵 | 中国科学院青岛生物能源与过程研究所, 生物燃料重点实验室, 青岛 266101 | | | 李明时 | 常州大学石油化工学院, 江苏省绿色催化材料与技术重点实验室, 常州 213164 | mingshili@cczu.edu.cn |
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| 摘要: 采用水热合成法使铁进入分子筛MFI骨架结构，成功合成出含骨架铁的分子筛Na-[Fe]-ZSM-5，并通过离子交换法负载Pt制备脱氢催化剂Pt/Na-[Fe]-ZSM-5。通过正十二烷脱氢反应，研究了该催化剂对长链烷烃脱氢制单烯烃反应的催化性能。采用N2吸附-脱附测试、X射线衍射（XRD）、傅立叶变换红外光谱（FT-IR）、氨气程序升温脱附（NH3-TPD）、吡啶吸附的红外光谱（Py-IR）、CO化学吸附、透射电子显微镜（TEM）等不同方法对催化剂进行了表征。结果表明，通过控制骨架铁含量可调控催化剂表面酸性；含骨架铁的ZSM-5分子筛载体具有抑制负载金属晶粒长大，保持金属高分散度的作用；其负载铂催化剂Pt/Na-[Fe]ZSM-5-50具有表面弱酸中心（0.69 mmol·g-1）和高分散Pt中心，因而具有良好的长链烷烃脱氢活性、稳定性和单烯烃选择；在转化率稳定在~20%时，TOF为4.56 s-1，单烯烃选择性为92.7%；在实验范围内，Pt/Na-[Fe]ZSM-5催化剂表面弱酸量和脱氢反应的本征活性（TOF）均随催化剂铁含量的增加而增加。 |
| 关键词: 沸石 模板合成 负载型催化剂 骨架铁 催化脱氢 酸性 |
| 基金项目: 国家自然基金（No.21761132006，21676029）资助项目。 |
| Abstract: The zeolite Na-[Fe]-ZSM-5 containing framework iron was successfully synthesized by hydrothermal synthesis, and the Pt/Na-[Fe]-ZSM-5 catalysts were prepared by ion exchange method. The catalytic performance of the catalysts for the dehydrogenation of long-chain alkanes to mono-olefin was investigated through the dehydrogenation of n-dodecane. The catalysts were characterized by N2 adsorption-desorption test, X-ray diffraction (XRD), Fourier transform infrared spectrum (FT-IR), NH3 temperature-programmed desorption (NH3-TPD), Ir spectra of pyridine adsorped (Py-IR), CO chemisorption and transmission electron microscope (TEM). The results show that the surface acidity of the catalyst can be adjusted by controlling the content of framework iron; the support, ZSM-5 containing framework iron, has the effect of inhibiting metal grain growth and maintaining high dispersion of metals; The Pt/Na-[Fe]-ZSM-5-50 catalyst had weak surface acid sites (0.69 mmol·g-1) and highly dispersed Pt sites, so it exhibited high activity and stability for the dehydrogenation and high selectivity of mono-olefin. When the conversion was stable at ~20%, the TOF was 4.56 s-1 and the selectivity of mono-olefin was 92.7%. In the experimental range, the amount of weak acid sites on the surface of Pt/Na-[Fe]-ZSM-5 catalyst and its intrinsic activity (TOF) of dehydrogenation increased with the increase of iron content. |
| Keywords: zeolites template synthesis supported catalysts framework iron catalytic dehydrogenation acidity |
| 投稿时间：2019-12-16 修订日期：2020-03-12 |
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| 崔孟涛,王忠,李学兵,李明时.含骨架铁ZSM-5的合成及其负载Pt催化剂在正十二烷脱氢反应中的催化性能[J].无机化学学报,2020,36(5):885-892. |
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