金属基离子液体催化生物质转化研究进展

doi:10.16085/j.issn.1000-6613.2020-0676

化工进展 ›› 2021, Vol. 40 ›› Issue (2): 800-812.DOI: 10.16085/j.issn.1000-6613.2020-0676

金属基离子液体催化生物质转化研究进展

马浩¹(), 蔡滔², 黄正宇², 陈利利¹, 乔艳辉¹, 滕俊江¹(), 纪红兵¹^,³

^1.广东石油化工学院化学学院，广东茂名 525000
^2.广东石油化工学院化学工程学院，广东茂名 525000
^3.中山大学化学学院精细化工研究院，广东广州 510275

收稿日期:2020-04-27 修回日期:2020-07-29 出版日期:2021-02-05 发布日期:2021-02-09
通讯作者: 滕俊江
作者简介:马浩（1985—），男，博士，副教授，研究方向为离子液体与生物质催化转化。E-mail：thma@gdupt.edu.cn。
基金资助:
国家自然科学基金(21808043);广东省自然科学基金(2018A030307055);广东省教育厅项目(2018KTSCX151);大学生创新创业项目(733283)

Catalytic conversion of biomass by metal-based ionic liquids

Hao MA¹(), Tao CAI², Zhengyu HUANG², Lili CHEN¹, Yanhui QIAO¹, Junjiang TENG¹(), Hongbing JI¹^,³

^1.College of Chemistry, Guangdong University of Petrochemical Technology, Maoming 525000, Guangdong, China
^2.College of Chemical Engineering, Guangdong University of Petrochemical Technology, Maoming 525000, Guangdong, China
^3.Fine Chemical Industry Research Institute, School of Chemistry, Sun Yat-sen University, Guangzhou 510275, Guangdong, China

Received:2020-04-27 Revised:2020-07-29 Online:2021-02-05 Published:2021-02-09
Contact: Junjiang TENG

摘要/Abstract

摘要：

生物质是自然界中含量丰富且唯一可再生的有机碳资源，可以经过化学反应转化为高附加值碳基化学品和燃料，被认为是传统化石资源的理想替代品。催化材料的设计开发是生物质资源开发和利用的关键所在，离子液体因其独特的可设计性，在生物质资源利用过程中得到广泛应用。鉴于金属活性中心的催化活性以及离子液体的可设计性，将金属活性中心引入离子液体中制备金属基离子液体催化剂在生物质领域受到广泛关注，并取得一定进展。基于上述背景，本文综述了近年来金属基离子液体催化剂在生物质催化转化过程中的研究进展，重点介绍金属氯化物型、多金属氧酸盐型金属基离子液体在生物质基碳水化合物、木质素催化转化制备平台化学品，以及油脂催化（转）酯化制备生物柴油方面的研究进展；同时还综述了金属螯合物型金属基离子液体以及离子液体金属盐在生物质催化转化方面的研究工作。此外，对金属基离子液体在生物质资源方面的应用进行了总结和展望，并对金属基离子液体催化剂的设计提出建议，以期有助于生物质资源的开发和利用。

关键词: 金属基离子液体, 生物质, 催化转化, 高值化利用, 平台化学品

Abstract:

Biomass is the unique renewable organic carbon resource with abundant reserves in nature. Through the reaction processes in the presence of a catalyst, it can be converted into high value-added carbon-based chemicals and fuels. Biomass has been considered as an ideal substitute for traditional fossil resources. The development of catalyst material plays the key roles in utilization of biomass resources. Ionic liquids (ILs), known as designable materials, have been widely applied in this field. In view of the catalytic performance of metal ions and the designability of ILs, the introduction of metal sites into IL’s structure to prepare the metal-based ILs catalysts has attracted widespread attention in the field of biomass utilization. Herein, based on the above background, this paper aimed to review the recent progress in the catalytic conversion of biomass under the metal-based ILs catalysts by focusing on the catalytic conversion of biomass-based carbohydrates and lignin into platform chemicals, and the catalytic (trans-) esterification of oleic acid or oil to prepare biodiesel in the presence of metal chloride-ILs and polyoxometalate-ILs, respectively. Meanwhile, the catalytic conversion of other biomass by the metal chelate-ILs and ILs metal salt was also reviewed. In addition, the application of metal-based ILs in biomass utilization field were summarized and prospected, and some suggestions were given to guide the design of metal-based ILs catalysts. Hopefully, it would be helpful in development and utilization of biomass resources.

Key words: metal-based ionic liquids, biomass, catalytic conversion, high value utilization, platform chemicals

中图分类号:

TQ352

马浩, 蔡滔, 黄正宇, 陈利利, 乔艳辉, 滕俊江, 纪红兵. 金属基离子液体催化生物质转化研究进展[J]. 化工进展, 2021, 40(2): 800-812.

Hao MA, Tao CAI, Zhengyu HUANG, Lili CHEN, Yanhui QIAO, Junjiang TENG, Hongbing JI. Catalytic conversion of biomass by metal-based ionic liquids[J]. Chemical Industry and Engineering Progress, 2021, 40(2): 800-812.

图/表 13

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催化剂	溶剂	原料	产物	反应条件		转化率 /%	产率 /%	参考文献
催化剂	溶剂	原料	产物	温度/℃	时间/h	转化率 /%	产率 /%	参考文献
H₃PW₁₂O₄₀	DMSO	果糖	HMF	120	2	97.9	96.7	[34]
[C₃H₆SO₃Hmim]₃PW₁₂O₄₀	DMSO	果糖	HMF	120	2	98.9	76.2	[34]
[C₃H₆SO₃Hmim]₃PW₁₂O₄₀	2-BuOH	果糖	HMF	120	2	99.7	99.1	[34]
H₃PW₁₂O₄₀	EtOH	果糖	乙酰丙酸乙酯	120	12	>99	84	[35]
[C₃H₆SO₃Hmim]₃PW₁₂O₄₀	EtOH	果糖	乙酰丙酸乙酯	120	12	>99	76	[35]
H₃PW₁₂O₄₀	H₂O/THF(1∶5)	葡萄糖	HMF	180	4	—	40.8	[36]
[SO₃HpyzH]HPW₁₂O₄₀	H₂O/THF(1∶5)	葡萄糖	HMF	180	5	—	46.4	[36]
H₃PW₁₂O₄₀	H₂O/THF(1∶2)	葡萄糖	HMF	160	7.5	约100	49.4	[38]
[C₂H₄NH₂mim]H₂PW₁₂O₄₀	H₂O/THF(1∶2)	葡萄糖	HMF	160	7.5	约100	53.9	[38]
H₃PW₁₂O₄₀	H₂O/MIBK(1∶1)	纤维素	葡萄糖	140	5	54.1	27.0	[39]
[C₃H₆SO₃Hmim]H₂PW₁₂O₄₀	H₂O/MIBK(1∶1)	纤维素	葡萄糖	140	5	55.1	36.0	[39]
H₃PW₁₂O₄₀	MeOH	纤维素	乙酰丙酸甲酯	150	5	100	29.7	[40]
[C₃H₆SO₃Hpy]₃PW₁₂O₄₀	MeOH	纤维素	乙酰丙酸甲酯	150	5	100	71.4	[40]

催化剂	溶剂	原料	产物	反应条件		转化率 /%	产率 /%	参考文献
催化剂	溶剂	原料	产物	温度/℃	时间/h	转化率 /%	产率 /%	参考文献
H₃PW₁₂O₄₀	DMSO	果糖	HMF	120	2	97.9	96.7	[34]
[C₃H₆SO₃Hmim]₃PW₁₂O₄₀	DMSO	果糖	HMF	120	2	98.9	76.2	[34]
[C₃H₆SO₃Hmim]₃PW₁₂O₄₀	2-BuOH	果糖	HMF	120	2	99.7	99.1	[34]
H₃PW₁₂O₄₀	EtOH	果糖	乙酰丙酸乙酯	120	12	>99	84	[35]
[C₃H₆SO₃Hmim]₃PW₁₂O₄₀	EtOH	果糖	乙酰丙酸乙酯	120	12	>99	76	[35]
H₃PW₁₂O₄₀	H₂O/THF(1∶5)	葡萄糖	HMF	180	4	—	40.8	[36]
[SO₃HpyzH]HPW₁₂O₄₀	H₂O/THF(1∶5)	葡萄糖	HMF	180	5	—	46.4	[36]
H₃PW₁₂O₄₀	H₂O/THF(1∶2)	葡萄糖	HMF	160	7.5	约100	49.4	[38]
[C₂H₄NH₂mim]H₂PW₁₂O₄₀	H₂O/THF(1∶2)	葡萄糖	HMF	160	7.5	约100	53.9	[38]
H₃PW₁₂O₄₀	H₂O/MIBK(1∶1)	纤维素	葡萄糖	140	5	54.1	27.0	[39]
[C₃H₆SO₃Hmim]H₂PW₁₂O₄₀	H₂O/MIBK(1∶1)	纤维素	葡萄糖	140	5	55.1	36.0	[39]
H₃PW₁₂O₄₀	MeOH	纤维素	乙酰丙酸甲酯	150	5	100	29.7	[40]
[C₃H₆SO₃Hpy]₃PW₁₂O₄₀	MeOH	纤维素	乙酰丙酸甲酯	150	5	100	71.4	[40]

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金属基离子液体催化生物质转化研究进展

Catalytic conversion of biomass by metal-based ionic liquids

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