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化学进展 2020, Vol. 32 Issue (12): 2034-2048 DOI: 10.7536/PC200424 前一篇   后一篇

• 综述 •

低共熔溶剂预处理木质纤维素生产生物丁醇

黄秉乾1, 王立艳1,**(), 韦漩2, 徐伟超1,2, 孙振1, 李庭刚2,3,**()   

  1. 1 中国矿业大学(北京)化学与环境工程学院 北京 100083
    2 中国科学院绿色过程制造创新研究院 中国科学院绿色过程与工程重点实验室 北京市过程污染控制工程技术研究中心 中国科学院过程工程研究所 北京 100190
    3 中国科学院大学 北京 100049
  • 收稿日期:2020-04-20 修回日期:2020-08-16 出版日期:2021-10-15 发布日期:2020-10-15
  • 通讯作者: 王立艳, 李庭刚
  • 作者简介:
    ** Corresponding author e-mail: (Liyan Wang); (Tinggang Li)
  • 基金资助:
    国家自然科学基金项目(No. 50978246); 水体污染控制与治理国家科技重大专项(No. 2017ZX07402001); 稀土产业基金项目(No. IAGM2020DB06)
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Lignocellulose Pretreatment by Deep Eutectic Solvents for Biobutanol production

Bingqian Huang1, Liyan Wang1,**(), Xuan Wei2, Weichao Xu1,2, Zhen Sun1, Tinggang Li2,3,**()   

  1. 1 School of Chemical and Environmental Engineering, China University of Mining and Technology, Beijing 100083, China
    2 Innovation Academy for Green Manufacture, CAS Key Laboratory of Green Process and Engineering, Beijing Engineering Research Center of Process Pollution Control, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
    3 University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2020-04-20 Revised:2020-08-16 Online:2021-10-15 Published:2020-10-15
  • Contact: Liyan Wang, Tinggang Li
  • Supported by:
    the National Natural Science Foundation of China(No. 50978246); the Research Fund of Major Science and Technology Program for Water Pollution Control and Treatment(No. 2017ZX07402001); and Rare Earth Industry Fund(No. IAGM2020DB06)

生物丁醇被认为是一种能够直接代替汽油的生物燃料,可满足经济发展对可持续液体燃料的需求。木质纤维素可再生,来源广泛且廉价,是生产生物丁醇的理想原料。但木质纤维素结构复杂,难以直接水解利用,高效的预处理方式是其商业化应用的关键。低共熔溶剂(DES)是一种环境友好的新型溶剂,具有成本低、绿色低毒、溶解能力强、良好的选择性和生物相容性等优点,有着较高的生物质预处理潜力。本文首先介绍了DES的种类和性质;其次,综述了木质纤维素中各组分在DES中的溶解效率,讨论了DES预处理木质纤维素对酶水解和丁醇发酵过程的影响;再次,通过对各种生物加工过程的梳理,对整合生物过程在生产生物丁醇领域的应用潜力进行了评述;最后,对DES预处理木质纤维素生产生物丁醇领域今后的工作做出了展望。

关键词： 低共熔溶剂, 预处理, 木质纤维素, 生物丁醇, 整合生物过程

Biobutanol is acknowledged as a direct alternative of gasoline, which can meet the demand of sustainable economic development for renewable liquid fuel. Lignocellulosic biomass is an ideal raw material for the biobutanol production due to its merits of being renewable, cheap and easily accessible. However, the complex structure of lignocellulose hinders its direct hydrolysis, and efficient pretreatment is essential for its commercial application. As a novel and environmentally friendly solvent, deep eutectic solvents(DESs) have high potential for biomass pretreatment due to its advantages of low cost, low toxicity, strong solubility, excellent selectivity and biocompatibility. This article mainly focuses on the application of DES in lignocellulose pretreatment for biobutanol production. Firstly, the types and properties of DESs are introduced. Secondly, the dissolution efficiency of components in lignocellulose in DESs is summarized, and the effects of DESs pretreatment on enzymatic hydrolysis and butanol fermentation process are discussed. Thirdly, the application potential of consolidated bioprocessing in the production of biobutanol is reviewed by combing various bioprocessing processes. Finally, the prospects of DESs pretreatment lignocellulose for producing biobutanol are proposed.

Contents

1 Introduction

2 DESs and their physicochemical properties

2.1 Classification of DESs

2.2 Properties of DESs

3 Lignocellulose pretreatment by DESs

3.1 Reducing recalcitrance of the lignocellulose by DESs

3.2 Analysis on Solubility of Lignocellulose Components in DESs

4 Effect of DES pretreatment on the production process of biobutanol

4.1 Effect of DES pretreatment on enzymatic hydrolysis

4.2 Effect of DES pretreatment on butanol fermentation

5 Consolidated bioprocessing of biobutanol

5.1 Continuous consolidation of production processes

5.2 Continuous exploration of consolidated bioprocessing

6 Recovery of lignin and recycling of DESs

6.1 Recovery of lignin

6.2 Recycling of DESs

7 Conclusion and prospectives

Key words: deep eutectic solvents, pretreatment, lignocellulose, biobutanol, consolidated bioprocessing
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图1 HBD与季铵盐氯化胆碱的相互作用[32]
Fig.1 Interaction of a HBD with the quaternary ammonium salt choline chloride[32]
图2 用于DES合成的氢键供体(HBDs)和氢键受体(HBAs)的典型结构[34]
Fig.2 Typical structures of hydrogen bond donors(HBDs) and bond acceptors(HBAs) for DES synthesis[34]
表1 一些常见的DES的熔点和黏度
Table 1 Freezing points and viscosity of some common DESs
HBA Freezing point(℃) HBD Freezing point
(℃) 		Molar ratio
(HBA∶HBD) 		Freezing point of DESs(℃) Viscosity of DESs(cP) ref
ChCl 303 Urea 134 1∶2 12 750(25 ℃) 36, 39
ChCl 303 Acetamide 80 1∶2 51 - 39
ChCl 303 Adipic acid 153 1∶1 85 - 39
ChCl 303 Citric acid 149 1∶1 69 - 39
ChCl 303 Malonic acid 134 1∶1 10 721(25 ℃) 36, 39
ChCl 303 Oxalic acid 190 1∶1 34 - 39
ChCl 303 Ethylene glycol -12.9 1∶2 -12.9 37(25 ℃) 36, 39
ChCl 303 Glycerol 17.8 1∶2 17.8 259(25 ℃) 36, 39
ChCl 303 Imidazole - 3∶7 56 15(70 ℃) 36, 39
ChCl 303 ZnCl 2 293 1∶2 - 85 000(25 ℃) 36, 39
ZnCl 2 293 Urea 134 1∶3.5 9 11 340(25 ℃) 36, 39
ZnCl 2 293 Acetamide 80 - -16 - 39
ZnCl 2 293 Ethylene glycol -12.9 - -30 - 39
图3 DES对木质纤维素的预处理[52]
Fig.3 Pretreatment of lignocellulose by DES[52]
表2 木质素和纤维素在各种DES中的溶解度
Table 2 Solubility of lignin and cellulose in various DESs
Biomass HBA HBD Molar ratio Pretreatment conditions Lignin removal
(%) 		Cellulose reservation(%) ref
Rice straw betaine Lactic acid 1∶2 60 ℃, 12 h 52 - 51
Rice straw betaine Lactic acid 1∶5 60 ℃, 12 h 56 - 51
Rice straw ChCl Lactic acid 1∶2 60 ℃, 12 h 51 - 51
Rice straw ChCl Lactic acid 1∶5 60 ℃, 12 h 60 - 51
Wheat straw ChCl Lactic acid 1∶2 90 ℃, 12 h 49 57.8 18
Wheat straw ChCl Citric acid 1∶1 90 ℃, 12 h 40.6 59.1 18
Wheat straw ChCl Acetic acid 1∶2 90 ℃, 12 h 32.1 63.2 18
Wheat straw ChCl Ethanolamine 1∶6 90 ℃, 12 h 81 90.8 18
Wheat straw ChCl Diethanolamine 1∶8 90 ℃, 12 h 73.5 98.0 18
Wheat straw ChCl Methyldiethanolamine 1∶10 90 ℃, 12 h 44.6 98.6 18
Wheat straw ChCl Urea 1∶2 90 ℃, 12 h 27.7 95.9 18
Wheat straw ChCl Glycerol 1∶2 90 ℃, 12 h 24.7 97.8 18
Wheat straw ChCl Ethylene glycol 1∶2 90 ℃, 12 h 12.2 95.7 18
Corncob ChCl 1,4-butanediol 1∶9 180 ℃, 4 h 95.02 98.59 20
Corncob ChCl Lactic acid 1∶2 70 ℃, 24 h 18.1 - 20
Corncob ChCl Lactic acid 1∶2 80 ℃, 24 h 31.1 - 20
Corncob ChCl Lactic acid 1∶2 90 ℃, 24 h 42.7 - 20
Corncob ChCl Lactic acid 1∶2 100 ℃, 24 h 65.8 - 20
Corncob ChCl Lactic acid 1∶2 110 ℃, 24 h 95.5 - 20
Corncob ChCl Lactic acid 1∶5 90 ℃, 24 h 77.9 - 20
Corncob ChCl Lactic acid 1∶10 90 ℃, 24 h 86.1 - 20
Corncob ChCl Lactic acid 1∶15 90 ℃, 24 h 93.1 - 20
Corncob ChCl Malonic acid 1∶1 90 ℃, 24 h 56.5 - 20
Corncob ChCl Glutaric acid 1∶1 90 ℃, 24 h 34.3 - 20
Corncob ChCl Malic acid 1∶1 90 ℃, 24 h 22.4 - 20
Corncob ChCl Ethylene glycol 2∶1 90 ℃, 24 h 87.6 - 20
Corncob ChCl Glycerol 2∶1 90 ℃, 24 h 71.3 - 20
Switchgrass ChCl 4-hydroxybenzyl alcohol 1∶1 160 ℃, 33 h 0.4 - 67
Switchgrass ChCl Catechol 1∶1 160 ℃, 33 h 49.0 - 67
Switchgrass ChCl Vanillin 1∶2 160 ℃, 33 h 52.5 - 67
Switchgrass ChCl P-coumaric 1∶1 160 ℃, 33 h 60.8 - 67
图4 DES预处理木质纤维素生产生物丁醇流程图
Fig.4 Flow chart of biobutanol production by lignocellulose pretreatment with DESs
表3 不同预处理条件下纤维素和木聚糖的转化率以及葡萄糖的产率
Table 3 Conversion rates of cellulose and xylan and yield of glucose under different pretreatment conditions
Biomass DES Pretreatment conditions Cellulose conversion(%) Xylan conversion(%) Glucose yield
(%) 		ref
Rice straw Untreated 120 ℃, 6 h 23.9 6.6 - 57
Rice straw Lac∶Ethylene glycol(1∶1) 120 ℃, 6 h 58.2 50.2 - 57
Rice straw Lac∶Glycerol(1∶1) 120 ℃, 6 h 56.4 26.0 - 57
Rice straw Lac∶Xylitol(1∶1) 120 ℃, 6 h 47.0 22.0 - 57
Rice straw Lac∶Formamide(1∶1) 120 ℃, 6 h 50.1 30.8 - 57
Rice straw Lac∶Urea(1∶1) 120 ℃, 6 h 23.4 6.5 - 57
Rice straw Lac∶Guanidine·HCl(1∶1) 120 ℃, 6 h 80.3 79.3 - 57
Rice straw ChCl∶Ethylene glycol(1∶1) 120 ℃, 6 h 33.9 10.1 - 57
Rice straw ChCl∶Glycerol(1∶1) 120 ℃, 6 h 30.2 8.7 - 57
Rice straw ChCl∶Xylitol(1∶1) 120 ℃, 6 h 27.8 6.6 - 57
Rice straw ChCl∶Formamide(1∶1) 120 ℃, 6 h 41.4 18.0 - 57
Rice straw ChCl∶Urea(1∶1) 120 ℃, 6 h 41.0 16.9 - 57
Rice straw ChCl∶Guanidine·HCl(1∶1) 120 ℃, 6 h 37.4 9.7 - 57
Rice straw ChCl∶Lac(1∶1) 80 ℃, 6 h 47.3 22.0 - 57
Rice straw ChCl∶2-Chloropropionic acid(1∶1) 80 ℃, 6 h 73.0 36.3 - 57
Rice straw ChCl∶Oxalic acid (1∶1) 80 ℃, 6 h 68.3 37.1 - 57
Wheat straw Untreated 90 ℃, 12 h 20.6 8.6 - 18
Wheat straw ChCl∶Lac(1∶2) 90 ℃, 12 h 93.9 69 - 18
Wheat straw ChCl∶Citric acid(1∶1) 90 ℃, 12 h 63.9 39.2 - 18
Wheat straw ChCl∶Acetic acid(1∶2) 90 ℃, 12 h 37.8 32.3 - 18
Wheat straw ChCl∶Ethanolamine(1∶6) 90 ℃, 12 h 92.4 75.8 - 18
Wheat straw ChCl∶Diethanolamine(1∶8) 90 ℃, 12 h ~75 ~51 - 18
Wheat straw ChCl∶Methyldiethanolamine(1∶10) 90 ℃, 12 h 51.6 38.0 - 18
Corncob Untreated 90 ℃, 24 h - - 22.1 20
Corncob ChCl∶Lac(1∶2) 90 ℃, 24 h - - 81.6 20
Corncob ChCl∶Lac(1∶5) 90 ℃, 24 h - - 83.5 20
Corncob ChCl∶Lac(1∶10) 90 ℃, 24 h - - 83.2 20
Corncob ChCl∶Lac(1∶15) 90 ℃, 24 h - - 79.1 20
Corncob ChCl∶Lac(1∶2) 70 ℃, 24 h - - 44.9 20
Corncob ChCl∶Lac(1∶2) 80 ℃,24 h - - 73.6 20
Corncob ChCl∶Lac(1∶2) 90 ℃, 24 h - - 79.7 20
Corncob ChCl∶Lac(1∶2) 100 ℃, 24 h - - 78.0 20
Corncob ChCl∶Lac(1∶2) 110 ℃, 24 h - - 77.8 20
Corncob Untreated - 32.8 15.5 - 75
Corncob ChCl∶Glycerol(1∶2) 80 ℃, 15 h 39.9 17.7 - 75
Corncob ChCl∶Glycerol(1∶2) 115 ℃, 15 h 79.1 61.3 - 75
Corncob ChCl∶Glycerol(1∶2) 150 ℃, 15 h 91.5 95.5 - 75
Corncob ChCl∶Imidazole(3∶7) 80 ℃, 15 h 92.3 59.5 - 75
Corncob ChCl∶Imidazole(3∶7) 115 ℃, 15 h 94.0 84.0 - 75
Corncob ChCl∶Imidazole(3∶7) 150 ℃, 15 h 94.6 84.8 - 75
表4 不同预处理条件下丁醇产量
Table 4 Butanol yield under different pretreatment conditions
Biomass Pretreatment method Fermentation time(h) Butanol yield
(g/L) 		total solvent yield
(g/L) 		ref
Glucose medium 1 - 65.5 8.7 12.3 76
Corn stover [Bmim][Cl] 50 7.4 11.7 76
Glucose medium 2 - 36 10 15.6 76
Corn stover ChCl∶Formic acid 49 5.6 7.0 76
Glucose medium 3 - 72 10.59 14.52 69
Rice straw ChCl∶Formic acid∶acetic acid 72 9.54 13.73 69
Glucose medium 4 - 72 10.23 16.87 69
Rice straw Ethylamine hydrochloride∶Lac 72 10.1 15.79 69
图5 木质纤维素转化为增值产品的各种生物加工选择[59]
Fig.5 Various bioprocessing options available for the conversion of lignocellulosic biomass to useful products[59]
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