磁性碱木素胺稳定的Ru纳米粒子催化α-蒎烯加氢反应

doi:10.7503/cjcu20200232

高等学校化学学报 ›› 2020, Vol. 41 ›› Issue (8): 1826.doi: 10.7503/cjcu20200232

磁性碱木素胺稳定的Ru纳米粒子催化α-蒎烯加氢反应

陈祥云¹, 朱本强¹, 袁冰¹, 于凤丽¹, 解从霞¹, 于世涛²

1. 生态化工国家重点实验室培育基地, 青岛科技大学化学与分子工程学院, 青岛 266042;
2. 青岛科技大学化工学院, 青岛 266042

收稿日期:2020-04-26 出版日期:2020-08-10 发布日期:2020-07-31
通讯作者: 袁冰,女,博士,教授,主要从事环境友好催化研究.E-mail:yuanbing@qust.edu.cn;解从霞,女,博士,教授,主要从事精细化学品的合成及性能研究.E-mail:xiecongxia@126.com E-mail:yuanbing@qust.edu.cn;xiecongxia@126.com
基金资助:
国家自然科学基金（批准号：31870554，31470595）、山东省重点研发计划项目（公益专项）（批准号：2017GGX40105）和山东省泰山学者项目（批准号：ts201511033）资助．

Hydrogenation of α-Pinene Catalyzed by Ru Nanoparticles Stabilized by Magnetic Alkali Lignin Amine

CHEN Xiangyun¹, ZHU Benqiang¹, YUAN Bing¹, YU Fengli¹, XIE Congxia¹, YU Shitao²

1. State Key Laboratory Base of Eco-chemical Engineering, College of Chemistry and Molecular Engineering, Qingdao 266042, China;
2. College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China

Received:2020-04-26 Online:2020-08-10 Published:2020-07-31
Supported by:
Supported by the the National Natural Science Foundation of China(Nos.31870554, 31470595), the Key R & D Plan of Shandong Province, China(No.2017GGX40105) and the Taishan Scholars Projects of Shandong Province, China(No.ts201511033).

1. ESM to 1826-1835.pdf(372KB)

摘要/Abstract

摘要： 通过Mannich反应在碱木素结构中引入胺源，再结合共沉淀法制备了包裹Fe₃O₄磁核的稳定金属粒子的碱木素胺载体，并进一步构建了催化可再生资源α-蒎烯加氢反应的Ru纳米粒子催化剂.通过元素分析、粉末X射线衍射、傅里叶变换红外光谱、电感耦合等离子体原子发射光谱、透射电子显微镜、热重分析和X射线光电子能谱等方法对该催化剂进行表征.结果表明，碱木素中的苯环和含氧基团均对金属粒子有稳定作用，但胺源的引入可更加有效地稳定金属粒子.经过对催化剂制备工艺、木质素类型、胺源类型和胺源含量的筛选，得到活性最优的催化剂Fe₃O₄@0.8ALN₁-Ru，Ru负载量为1.92 mmol/g，Ru粒子粒径为（2.1±0.5）nm.该催化剂在n（α-蒎烯）/n（Ru）=65.8，1 MPa H₂条件下70℃催化1 mL α-蒎烯加氢反应2 h，可获得99.64%的α-蒎烯转化率和96.52%的顺式蒎烷选择性，并表现出良好的重复使用稳定性.

关键词: 碱木素胺, 纳米粒子, α-蒎烯, 加氢反应

Abstract: Alkali lignin amine was prepared by introducing amine into alkali lignin structure via Mannich reaction to improve the stability performance for metal nanoparticles. Then the alkali lignin amine was wrapped around Fe₃O₄ magnetic nucleus by co-precipitation method and used as a carrier to construct Ru metal nanoparticle catalyst for hydrogenation of α-pinene. Elemental analysis(EA), X-ray diffraction(XRD), Fourier transform infrared(FTIR), inductively coupled plasma-atomic emission spectroscopy(ICP-AES), transmission electron microscope(TEM), thermogravimetric analysis(TG), X-ray photoelectron spectroscopy(XPS) and other characterizations showed that except for the benzene ring and oxygen-containing groups in alkali lignin, the introduced amine source had exhibited more efficient stabilization for metal nanoparticles. Fe₃O₄@0.8ALN₁-Ru, with a Ru loading of 1.92 mmol/g and Ru particle size of (2.1±0.5) nm, was found the most active catalyst of α-pinene hydrogenation after the study on catalyst preparation process, lignin type, amine source type and amine content. It exhibited a good catalytic performance with 99.64% conversion of α-pinene and 96.52% selectivity for cis-pinene when it catalyzed 1 mL of α-pinene and 1 MPa H₂ at a dosage of 0.05 g and 70℃ for 2 h. Moreover, it's good reuse stability confirmed by a five-run test, which provides a novel method for the development of high value-added lignin-based catalysts.

Key words: Alkali lignin amine, Nanoparticles, α-Pinene, Hydrogenation

中图分类号:

TrendMD:

陈祥云, 朱本强, 袁冰, 于凤丽, 解从霞, 于世涛. 磁性碱木素胺稳定的Ru纳米粒子催化α-蒎烯加氢反应. 高等学校化学学报, 2020, 41(8): 1826.

CHEN Xiangyun, ZHU Benqiang, YUAN Bing, YU Fengli, XIE Congxia, YU Shitao. Hydrogenation of α-Pinene Catalyzed by Ru Nanoparticles Stabilized by Magnetic Alkali Lignin Amine. Chem. J. Chinese Universities, 2020, 41(8): 1826.

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磁性碱木素胺稳定的Ru纳米粒子催化α-蒎烯加氢反应

Hydrogenation of α-Pinene Catalyzed by Ru Nanoparticles Stabilized by Magnetic Alkali Lignin Amine

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