Preparation and performance of Zn/H-ZSM-5 catalyst for catalytic amination of allyl alcohol to 3-picoline

MA Tianqi; WEI Tianyu; PIAN Yanjie; ZHANG Yuecheng; ZHAO Jiquan

doi:10.3969/j.issn.0438-1157.2014.03.020

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Preparation and performance of Zn/H-ZSM-5 catalyst for catalytic amination of allyl alcohol to 3-picoline

更新时间：2025-12-10

- Preparation and performance of Zn/H-ZSM-5 catalyst for catalytic amination of allyl alcohol to 3-picoline
- CIESC Journal Issue 3, Pages: 905-911(2014)
- 作者机构：
  
  河北工业大学化工学院,天津,300130
- 作者简介：
- 基金信息：
- DOI：10.3969/j.issn.0438-1157.2014.03.020
  CLC： TQ032.4}
- Online First：05 March 2014，
  
  Published：05 March 2014
- 稿件说明：
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MA Tianqi, WEI Tianyu, PIAN Yanjie, et al. Preparation and performance of Zn/H-ZSM-5 catalyst for catalytic amination of allyl alcohol to 3-picoline[J]. CIESC Journal, 2014, (3): 905-911.
DOI：

MA Tianqi, WEI Tianyu, PIAN Yanjie, et al. Preparation and performance of Zn/H-ZSM-5 catalyst for catalytic amination of allyl alcohol to 3-picoline[J]. CIESC Journal, 2014, (3): 905-911. DOI： 10.3969/j.issn.0438-1157.2014.03.020.

摘要

采用浸渍法制备了一系列H-ZSM-5分子筛负载过渡金属锌催化剂，在固定床反应器上考察了这些催化剂对丙烯醇催化氨化合成3-甲基吡啶的催化性能。通过对H-ZSM-5的硅铝比、锌负载量对催化剂催化性能影响的考察，发现硅铝比为80、锌负载量为12%时得到的催化剂Zn12/H-ZSM-5（80）的催化性能最佳。在常压、反应温度420℃、氨醇摩尔比3：1、空速300 h-1条件下，丙烯醇在该催化剂上的转化率和3-甲基吡啶的选择性分别达到97.8%和37.9%。利用X射线衍射（XRD）、X射线光电子能谱（XPS）以及吡啶吸附红外对催化剂进行了表征，结果表明，Zn12/H-ZSM-5（80）上负载的Zn2+为L酸；在丙烯醇生成3-甲基吡啶的反应过程中催化剂的脱氢活性物种为氧化锌，而加成和环合反应则主要是由催化剂中的L酸催化实现的。

Abstract

H-ZSM-5 supported zinc catalysts were prepared by impregnation method

and their catalytic performances for amination of allyl alcohol to 3-picoline were evaluated in a fixed-bed reactor. It is found that the catalyst Zn12/H-ZSM-5(80) (H-ZSM-5 with 80 silicon/aluminum (Si/Al) ratio and zinc loading of 12%) shows the best performance among all the studied catalysts. 97.8% conversion of allyl alcohol and 37.9% selectivity toward 3-picoline are obtained on this catalyst using reaction conditions: atmospheric pressure

at 420℃

ammonia/allyl alcohol mole ratio 3:1 and gas hour space velocity 300 h-1. The characterization results

obtained by X-ray diffraction (XRD)

X-ray photoelectron spectroscopy (XPS) and FT-IR of absorbed pyridine

indicate that zinc on Zn12/H-ZSM-5(80) is Zn2+

there is Lewis acid on HZSM-5. In 3-picoline formation

ZnO provides active sites of dehydrogenation reaction

and addition and cyclization reactions are mainly catalyzed by the Lewis acid.

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