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Progress in Chemistry 2020, Vol. 32 Issue (12): 2034-2048 DOI: 10.7536/PC200424 Previous Articles   Next Articles

• Review •

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: Revised: Online: Published:
  • 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)
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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
Fig.1 Interaction of a HBD with the quaternary ammonium salt choline chloride[32]
Fig.2 Typical structures of hydrogen bond donors(HBDs) and bond acceptors(HBAs) for DES synthesis[34]
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
Fig.3 Pretreatment of lignocellulose by DES[52]
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
Fig.4 Flow chart of biobutanol production by lignocellulose pretreatment with DESs
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
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
Fig.5 Various bioprocessing options available for the conversion of lignocellulosic biomass to useful products[59]
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