Advances on catalysts and solvents for catalytic hydrogenolysis of lignin

doi:10.16085/j.issn.1000-6613.2024-0469

Abstract

Abstract:

Biomass is a potential alternative resource for fossil fuels, and lignin is the second largest abundant reserves of biomass resource in nature. The catalytic conversion of lignin into high value-added chemicals is of great significance for the implementation of the national dual carbon strategy. Catalysts and solvents are key factors affecting the catalytic conversion of lignin. This article outlines the mechanisms and performance control laws of commonly used metals, molecular sieves, and metal oxide catalysts in the process of catalytic hydrogenation of lignin. Different solvent dispersion and hydrogen supply are compared and analyzed. Through in-situ characterization of solvent effects and simulation of solvent reaction pathways, the structure-activity relationship between catalyst structure and performance is explored, clarifying the synergistic mechanism of catalysts and solvents on lignin catalytic hydrogenation, providing a theoretical basis for the resource utilization and high-value utilization of lignin.

Key words: lignin, hydrodeoxygenation, catalysts, solvent, high-valued utilization

摘要：

生物质是化石能源的潜在替代资源，木质素是自然界第二大生物质资源，将木质素催化转化为高附加值化学品对国家“双碳”战略实施具有重要的意义。催化剂和溶剂是影响木质素催化转化反应过程的关键因素，本文概述了催化氢解木质素过程中常用的金属、分子筛和金属氧化物催化剂的作用机理以及性能调控规律，并对不同溶剂分散和供氢作用进行了对比分析，通过溶剂效应原位表征、溶剂反应路径模拟，探究催化剂结构和性能间的构效关系，明晰催化剂与溶剂对木质素催化氢解的协同作用机制，为木质素的资源化和高值化利用提供了理论基础。

关键词: 木质素, 加氢脱氧, 催化剂, 溶剂, 高值化利用

CLC Number:

TQ35

HAN Hongjing, CHE Yu, TIAN Yuxuan, WANG Haiying, ZHANG Yanan, CHEN Yanguang. Advances on catalysts and solvents for catalytic hydrogenolysis of lignin[J]. Chemical Industry and Engineering Progress, 2024, 43(S1): 315-324.

韩洪晶, 车宇, 田宇轩, 王海英, 张亚男, 陈彦广. 木质素催化氢解催化剂及溶剂的研究进展[J]. 化工进展, 2024, 43(S1): 315-324.

Figures/Tables 7

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反应物	溶剂	催化剂	反应条件	主产物收率	参考文献
2-苯氧基-1-苯乙醇	水	PdNi₄/MIL-100(Fe)	180℃、6h	酚类、酮类（81%）	[45]
桦木木质素	水	PdNi₄/MIL-100(Fe)	180℃、6h	酚类、酮类（17%）	[45]
愈创木酚	甲醇	SiO₂-Al₂O₃	400℃、1h	芳烃（57.93%）	[50]
2-(2-甲氧基苯氧基)- 1-苯基乙醇	超临界甲醇	Cu/CuMgAlO _x	300℃、4h	乙苯（100%）愈创木酚（96%）	[32]
苄基苯醚	乙醇	NiCu/Al₂O₃	200℃、2h	—	[54]
苄基苯醚	异丙醇	NiCu/Al₂O₃	200℃、2h	甲苯（100%）环己醇（100%）	[54]
苄基苯醚	叔丁醇	NiCu/Al₂O₃	200℃、2h	—	[54]
苄基苯醚	2-丁醇	NiCu/Al₂O₃	200℃、2h	甲苯（52.34%）苯酚（4.15%）环己醇（48.19%）	[54]
硫酸盐木质素	甲酸	Ni/沸石分子筛	200℃、3h	生物油（93.5%±4.1%）	[57]
香兰素	异丙醇	PdNi/CuFe₂O₄	180℃、3h	环己醇（95.8%）	[53]
硫酸盐木质素	异丙醇	Ni-Cu/H-Beta	330℃、3h	环烷烃（50.83%）	[24]
硫酸盐木质素	1,4二烷/甲醇/异丙醇	MoO₃-350	280℃、6h	石油醚可溶性产物[87%（质量分数）]	[59]
碱木质素	1,4二烷/乙醇/水	Pd/C NaOH	260℃、4h	苄醇[26.25%（质量分数）]	[60]
碱木质素	甲酸/异丙醇	WO₃-Al₂O₃	240℃、8h	生物油（63.4%）	[37]
玉米秸秆木质素	甲酸/异丙醇/水	Co/AC-N	235℃、200min	酚类化合物（23.8%）	[62]
杨木木质素	乙醇/异丙醇	NiCu/C	270℃、4h	单酚含量63.4%（质量分数）	[63]

反应物	溶剂	催化剂	反应条件	主产物收率	参考文献
2-苯氧基-1-苯乙醇	水	PdNi₄/MIL-100(Fe)	180℃、6h	酚类、酮类（81%）	[45]
桦木木质素	水	PdNi₄/MIL-100(Fe)	180℃、6h	酚类、酮类（17%）	[45]
愈创木酚	甲醇	SiO₂-Al₂O₃	400℃、1h	芳烃（57.93%）	[50]
2-(2-甲氧基苯氧基)- 1-苯基乙醇	超临界甲醇	Cu/CuMgAlO _x	300℃、4h	乙苯（100%）愈创木酚（96%）	[32]
苄基苯醚	乙醇	NiCu/Al₂O₃	200℃、2h	—	[54]
苄基苯醚	异丙醇	NiCu/Al₂O₃	200℃、2h	甲苯（100%）环己醇（100%）	[54]
苄基苯醚	叔丁醇	NiCu/Al₂O₃	200℃、2h	—	[54]
苄基苯醚	2-丁醇	NiCu/Al₂O₃	200℃、2h	甲苯（52.34%）苯酚（4.15%）环己醇（48.19%）	[54]
硫酸盐木质素	甲酸	Ni/沸石分子筛	200℃、3h	生物油（93.5%±4.1%）	[57]
香兰素	异丙醇	PdNi/CuFe₂O₄	180℃、3h	环己醇（95.8%）	[53]
硫酸盐木质素	异丙醇	Ni-Cu/H-Beta	330℃、3h	环烷烃（50.83%）	[24]
硫酸盐木质素	1,4二烷/甲醇/异丙醇	MoO₃-350	280℃、6h	石油醚可溶性产物[87%（质量分数）]	[59]
碱木质素	1,4二烷/乙醇/水	Pd/C NaOH	260℃、4h	苄醇[26.25%（质量分数）]	[60]
碱木质素	甲酸/异丙醇	WO₃-Al₂O₃	240℃、8h	生物油（63.4%）	[37]
玉米秸秆木质素	甲酸/异丙醇/水	Co/AC-N	235℃、200min	酚类化合物（23.8%）	[62]
杨木木质素	乙醇/异丙醇	NiCu/C	270℃、4h	单酚含量63.4%（质量分数）	[63]

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