钴-桔皮炭氢转移催化剂的制备及其催化加氢性能研究

doi:10.3969/j.issn.1673-5854.2021.04.003

生物质化学工程 ›› 2021, Vol. 55 ›› Issue (4): 14-20.doi: 10.3969/j.issn.1673-5854.2021.04.003

钴-桔皮炭氢转移催化剂的制备及其催化加氢性能研究

赵红叶¹^,², 邬怡¹, 杜政江¹, 刘全生¹, 周华从¹^,*()

1. 内蒙古工业大学化工学院, 内蒙古自治区低阶碳质资源高值功能化利用重点实验室, 内蒙古呼和浩特 010051
2. 内蒙古师范大学化学与环境科学学院, 内蒙古呼和浩特 010022

收稿日期:2020-07-17 出版日期:2021-07-30 发布日期:2021-07-10
通讯作者: 周华从 E-mail:hczhou@imut.edu.cn
作者简介:周华从, 教授, 博士, 硕士生导师, 研究领域: 低阶碳质资源高值化利用; E-mail: hczhou@imut.edu.cn
赵红叶(1983-), 女, 内蒙古乌兰察布人, 讲师, 博士, 主要从事生物质转化利用研究工作
基金资助:
中国科学院"西部之光"青年学者项目(2020ZY0010);国家自然科学基金资助项目(21968021);内蒙古师范大学引进高层次人才科研启动经费项目(2020YJRC018)

Preparation and Hydrogenation Performance of Cobalt-orange Peel Carbon Hydrogen Transfer Catalyst

Hongye ZHAO¹^,², Yi WU¹, Zhengjiang DU¹, Quansheng LIU¹, Huacong ZHOU¹^,*()

1. College of Chemical Engineering, Inner Mongolia University of Technology, Inner Mongolia Key Laboratory of High-Value Functional Utilization of Low Rank Carbon Resources, Hohhot 010051, China
2. College of Chemistry and Environmental Science, Inner Mongolia Normal University, Hohhot 010022, China

Received:2020-07-17 Online:2021-07-30 Published:2021-07-10
Contact: Huacong ZHOU E-mail:hczhou@imut.edu.cn

摘要/Abstract

摘要：

以生物质废弃物桔皮为原料，先热解制备桔皮炭材料，然后以桔皮炭为载体采用一步液相还原法制备钴-桔皮炭（Co-桔皮炭）催化剂，并将其应用于乙酰丙酸乙酯（EL）转化制备γ-戊内酯（GVL）反应。采用SEM、XRD、FT-IR、TG等技术对催化剂进行表征，结果显示：钴粒子均匀分布在炭载体表面，粒径约为0.1~2 μm，桔皮炭载体富含含氧结构。在以异丙醇为液体氢源、催化剂用量0.2 g、反应温度160℃和反应时间5 h的最佳加氢反应条件下，热解温度300℃制备的钴负载量20%的Co-桔皮炭作为氢转移催化剂对EL转化制备GVL具有良好催化效果，EL转化率高达99.3%，GVL得率为85.2%；Co-桔皮炭重复使用4次后其催化性能有所下降。

关键词: 桔皮, 氢转移催化剂, 催化加氢, 乙酰丙酸乙酯, γ-戊内酯

Abstract:

The biomass waste orange peel was used as raw material to prepare orange peel carbon material by pyrolysis. Then, the cobalt-orange peel carbon catalyst was constructed by one-step liquid phase reduction method with orange peel carbon as the support. The catalyst was used to catalyze the conversion of ethyl levulinate (EL) to γ-valerolactone(GVL).The catalysts were characterized by SEM, XRD, FT-IR and TG. The results showed that the cobalt particles were uniformly distributed on the surface of the carbon support, with the particle size of 0.1-2 μm. The orange peel carbon support was rich in oxygen-containing structure. The Co-orange peel carbon catalyst prepared at 300℃ with the loading amount of Co 20% was used as hydrogen transfer catalyst and had good catalytic effect and stability for the conversion of EL to GVL. After 5 h reaction at 160℃ with isopropanol as liquid hydrogen source, the conversion of EL was up to 99.3%, and the yield of GVL was 85.2%. The catalytic performance decreased after reused for 4 times.

Key words: orange peel, hydrogen transfer catalyst, catalytic hydrogenation, ethyl levulinate, γ-valerolactone

中图分类号:

TQ35

赵红叶, 邬怡, 杜政江, 刘全生, 周华从. 钴-桔皮炭氢转移催化剂的制备及其催化加氢性能研究[J]. 生物质化学工程, 2021, 55(4): 14-20.

Hongye ZHAO, Yi WU, Zhengjiang DU, Quansheng LIU, Huacong ZHOU. Preparation and Hydrogenation Performance of Cobalt-orange Peel Carbon Hydrogen Transfer Catalyst[J]. Biomass Chemical Engineering, 2021, 55(4): 14-20.

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循环次数/次 number of cycles	GVL得率/% yield of GVL	EL转化率/% conversion of EL	GVL选择性/% selectivity of GVL
1	36.8	63.3	58.2
2	34.5	59.6	57.8
3	31.2	53.0	58.9
4	8.4	23.6	35.5

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钴-桔皮炭氢转移催化剂的制备及其催化加氢性能研究

Preparation and Hydrogenation Performance of Cobalt-orange Peel Carbon Hydrogen Transfer Catalyst

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