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Progress in Chemistry 2022, Vol. 34 Issue (2): 285-300 DOI: 10.7536/PC210116 Previous Articles   Next Articles

• Review •

Applications of Lignin-Derived Porous Carbons for Electrochemical Energy Storage

Caiwei Wang1,2, Dongjie Yang1,2(), Xueqing Qiu3,4, Wenli Zhang3,4   

  1. 1 School of Chemistry and Chemical Engineering, South China University of Technology,Guangzhou 510640, China
    2 Guangdong Provincial Engineering Research Center for Green Fine Chemicals,Guangzhou 510640, China
    3 School of Chemical Engineering and Light Industry, Guangdong University of Technology,Guangzhou 510006, China
    4 Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, Guangdong University of Technology,Guangzhou 510006, China
  • Received: Revised: Online: Published:
  • Contact: Dongjie Yang
  • Supported by:
    National Key Research and Development Program of China(2018YFB1501503); National Natural Science Foundation of China(22038004); National Natural Science Foundation of China(21878114); Research and Development Program in Key Fields of Guangdong Province(2020B1111380002); Natural Science Foundation of Guangdong Province(2017A030308012); Natural Science Foundation of Guangdong Province(2018B030311052)
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Lignin is a renewable resource with the advantages of low cost, high carbon content, high aromaticity and easy collection. Lignin is regarded as one of the most important raw carbonaceous materials for industry to prepare new porous carbon materials in a large scale. It is of great strategic significance to alleviate the consumption of fossil fuel resources and deepen the sustainable development. Porous carbon materials have an extraordinary application prospect in the fields of energy storage materials, because of their high conductivity, high specific surface area, abundant porosity, excellent stability, etc. In this review, the latest research advances and developments for the preparation of lignin-derived porous carbon materials (LPCM) by template, activation and hydrothermal methods are reviewed pivotally. Meanwhile, the influences of pyrolysis parameters on the micro-structure of LPCM are summarized in detail. Furthermore, the applications of LPCM as the electrode materials for lithium-ion batteries, sodium-ion batteries and supercapacitors are illustrated emphatically. However, there exist some bottlenecks that the preparation processes of LPCM are complicated and their energy storage performances are relatively poor. Thus, the optimization of ion/electron diffusion kinetics, the synergistic effect of multiple energy storage mechanisms and the development of the green and facile preparation processes are proposed to conquer these challenges. The development of advanced carbonization techniques to construct the reasonable hierarchical porous structure, precise regulating the suitable interlayer spacing and the highly ordered arrangement of carbon layers, functionally modifying surface microenvironment, and the direct establishment of the relationship between carbonization parameters and electrochemical performance are the research directions to prepare LPCM with the high energy storage performances in the future.

Contents

1 Introduction

2 Preparation of lignin-derived porous carbon materials (LPCM)

2.1 Activation methods

2.2 Template methods

2.3 Hydrothermal method

3 Applications of LPCM in energy storage materials

3.1 Lithium-ion batteries

3.2 Sodium-ion batteries

3.3 Supercapacitors

4 Conclusion and outlook

Key words: lignin, preparation, carbon materials, lithium-ion batteries, sodium-ion batteries, supercapacitors
Table 1 Structural properties of LPCM prepared by direct carbonization and physical activation
Raw materials/
Preparation methods		 Temperature
(℃)		 Heating rate
(℃/min)		 Specific surface area (m2/g) Pore volume (cm3/g) Total pore volume (cm3/g) ref
Micropore Mesopore Macropore
Alkali lignin/Direct
carbonization		 900 1 529 0.21 0.04 - - 12
2 393 0.15 0.02
10 30 - 0.03
350 1 23 0.01 - - - 13
450 213 0.09
550 496 0.22
800 463 0.21
900 278 0.14
350 15 33.18 0.01 0.10 - - 14
450 52.31 0.01 0.13
550 56.35 0.02 0.13
600 57.74 0.02 0.14
Organosolv lignin/
Direct carbonization		 400 - 1.32 - - - 0.01 15
500 0.85 0.01
700 448.10 0.22
1000 432.33 0.23
Enzymatic hydrolysis
lignin/Steam activation		 700 - - 0.33 0.16 - 1.56 16
750 - 812 0.27 - - 0.30 17
800 - 865 0.37 0.26 - - 18
Alkali lignin/CO2
activation		 550 - 1343 - 0.10 0.51 - 13
800 1360 0.74 0.34
800 10 1613 - 0.77 0.31 - 19
850 1853 0.86 0.53
Table 2 Structural properties of LPCM prepared by chemical activation
Raw materials/
Preparation methods		 Temperature
(℃)		 Ratio (w/w) Heating rate ( ℃/min) Specific surface area (m2/g) Pore volume (cm3/g) Total pore volume (cm3/g) ref
Micropore Mesopore
Alkali lignin/KOH activation 750 1:1 10 1441 0.44 - 0.72 20
1:3 2714 0.73 1.31
1:4 2763 0.68 1.32
1:5 1582 0.28 0.82
550 1:3 10 959 0.34 - 0.49
650 1576 0.57 0.73
850 1390 0.30 0.70
650 1:3 25 2420 - - - 21
750 2940
850 2620
700 1:1 10 1250 - - - 22
800 1510
900 1350
700 4:1 3 514 0.21 0.03 0.25 23
Alkali lignin/
K2CO3 activation		 700 1:1 10 1640 - - - 22
800 1900
900 1650
Alkali lignin/ZnCl2 activation 350 1:1 10 534 0.21 0.03 0.36 24
400 1297 0.52 0.10 0.73
500 1347 0.63 0.15 0.93
600 1153 0.48 0.02 0.70
Fig. 1 Schematic diagram of LPCM prepared by hard template
Fig. 2 Schematic diagram of flower-like LPCM prepared by hard template using lamellar MgO[37]
Fig. 3 Schematic diagram of LPCM prepared by soft template[38]
Fig. 4 Schematic diagram of LPCM prepared by dual templates[36]
Table 3 Performances of LPCM anodes in lithium-ion batteries
Raw materials Preparation conditions Capacity (mAh/g) ref
Alkali lignin/KOH Lignin:KOH=5:2, 700 ℃, 2 h, N2, 10 ℃/min 470 (400 cycles at 0.2 A/g) 52
Enzymatic hydrolysis lignin/K2CO3 Lignin:K2CO3=1:1, 250 ℃, 0.5 h; 900 ℃, 2 h, N2 494 (200 cycles at 0.2 A/g) 53
Enzymatic hydrolysis lignin 300 ℃, 2 h; 800 ℃, 1 h, N2; 800 ℃, >1 h, H2 222 (200 cycles at 2 C) 54
Enzymatic hydrolysis lignin/K2CO3 Lignin:K2CO3=1:1, 250 ℃, 0.5 h; 900 ℃, 2 h, N2; 800 ℃,
1 h, H2		 520 (200 cycles at 0.2 A/g) 55
Enzymatic hydrolysis lignin/ZnCO3 Lignin:ZnCO3=1:1, 600 ℃, 2 h, N2 550 (200 cycles at 0.2 A/g) 56
Alkali lignin/SiO2 Lignin:SiO2=1:1, ball-milling, 600 ℃, 2 h, 2 ℃/min 900 (250 cycles at 0.2 A/g) 57
Alkali lignin/SiO2 Lignin:SDBS:SiO2=1:1:1, 250 ℃, 0.5 h; 600 ℃, 2 h, N2,
10 ℃/min		 1109 (100 cycles at 0.1 A/g) 58
Fig. 5 (a) Schematic diagram of LPCM prepared by ZnCO3, (b, c) TEM images of HLPC-ZnCO3-600, (d) Cycling performance of HLPC-ZnCO3-600 at 0.2 A/g, (e) Rate performance of HLPC-ZnCO3-600[56]
Fig. 6 (a) Schematic diagram of SiO2@LPCM prepared by dual templates, (b, c) SEM images of LHC/SiO2-21, (d) TEM image of LHC/SiO2-21, (e) Cycling performance of LHC/SiO2-21 at 0.1 A/g, (f) Rate performance of LHC/SiO2-21[58]
Table 4 Performances of lignin-derived hard carbon anodes in sodium-ion batteries
Raw materials Preparation conditions Capacity (mAh/g) ref
Alkali lignin 700/800/900 ℃, 2 h, 5 ℃/min, Ar 159/195/250 (5 cycles at 1/15 C) 66
Alkali lignin 1000 ℃, 2 ℃/min, N2 180 (200 cycles at 0.05 A/g) 67
Alkali lignin/Lignosulfonates 1200 ℃, 1 h, 5 ℃/min, Ar 200/120 (50 cycles at 1/10 C) 68
Lignosulfonates 600 ℃, 1 h; 1200 ℃, 1 h, 5 ℃/min, Ar 270 (50 cycles at 1/10 C)
Enzymatic hydrolysis lignin 900/1300 ℃, 10 ℃/min, N2 157/297 (100 cycles at 0.05 A/g ) 69
Alkali lignin/SiO2 (100 nm) 700 ℃, 4 h, 5 ℃/min, N2 100 (1000 cycles at 1 A/g ) 70
Fig. 7 (a) Schematic diagram of hard carbon prepared from alkali lignin and sodium lignosulphonate, (b) SEM image of alkali lignin derived hard carbon, (c) SEM image of sodium lignosulphonate derived hard carbon, (d) TEM image of alkali lignin derived hard carbon, (e) Initial coulombic efficiency, (f) Cycling performances at 1/10 C[68]
Fig.8 (a, b) SEM and TEM images of lignin-derived hard carbon prepared at 900 ℃ and 1300 ℃, (c) Cycling performances at 0.05 A/g, (d) Rate performances[69]
Fig. 9 Evolution of sodium-ion storage mechanisms in hard carbon prepared at different temperature[78]
Table 5 Performances of LPCM electrodes in supercapacitors
Raw materials Preparation conditions Specific surface area (m2/g) Total pore
volume (cm3/g)		 Capacity (F/g) Scan rate (A/g) Electrolyte ref
Alkali lignin/KOH Carbonization at 600 ℃, 1 h; lignin char:KOH=1:3, activation at 800 ℃, 2 h 2223 1.06 276 1 6 M KOH 84
Alkali lignin/KOH Carbonization at 500 ℃, 1 h; lignin char:KOH=1:4, activation at 800 ℃, 1 h 3775 2.70 287 0.2 6 M KOH 85
Organosolv lignin/
KOH		 Carbonization at 400 ℃, 1 h; Lignin:KOH=1:3, activation at 700 ℃, 1 h, 10 ℃/min 2265 - 336 1 6 M KOH 86
Enzymatic hydrolysis lignin/KOH Hydrothermal pretreatment at 200 ℃, 24 h; hydrothermally treated lignin:KOH=1:2, activation at 800 ℃, 1 h, 3 ℃/min 2218 - 312 1 6 M KOH 50
Enzymatic hydrolysis lignin/KOH Hydrothermal pretreatment at 180 ℃, 18 h, hydrothermally treated lignin:KOH=1:2, activation at 800 ℃, 1 h, 5 ℃/min 1660 0.78 420 0.1 6 M KOH 87
Sodium lignosulphonate Carbonization at 700 ℃, 1 h, 5 ℃/min 903 0.53 247 0.05 7 M KOH 85
Sodium lignosulphonate Pre-oxidation at 120 ℃, 2 h, 5 ℃/min, 200 ℃, 4 h, 0.5 ℃/min; carbonization at 700 ℃, 1 h, 5 ℃/min 1255 0.87 276 0.1 7 M KOH 89
Alkali lignin Carbonization at 400 ℃, 1 h, 2 ℃/min; 700 ℃, 1 h, 4 ℃/min 1269 0.60 245 0.2 6 M KOH 90
Alkali lignin/F127 Lignin:F127=45:72, Carbonization at 400 ℃, 1 ℃/min; 1000 ℃, 15 min, 2 ℃/min 185 0.28 77.1 - 6 M KOH 88
Alkali lignin/F127/CO2 Lignin:F127=45:72, Carbonization at 400 ℃, 1 ℃/min; 1000 ℃, 15 min, 2 ℃/min, activation at 875 ℃, 4 L/min 624 0.73 102.3 6 M KOH
Alkali lignin/F127/KOH Lignin:F127=45:72, carbonization at 400 ℃, 1 ℃/min; 1000 ℃, 15 min, 2 ℃/min, lignin/F127:KOH=1:2, activation at 1000 ℃, 10 ℃/min 1148 1.00 91.7 6 M KOH
Sodium lignosulphonate/ZnC2O4 Lignin:ZnC2O4=1:2, carbonization at 650 ℃, 2 h, 5 ℃/min 1069 406 320 1 6 M KOH 91
Fig. 10 (a) Schematic diagram of LPCM prepared by hydrothermal treatment and KOH activation, (b) SEM image, (c) Rate performance, (d) Performance of assembled symmetric supercapacitor[87]
Fig. 11 (a) Schematic diagram of LPCM prepared by gas exfoliation and in-situ ZnO template method, (b) SEM image of PLC-650-2, (c, d ) TEM images of PLC-650-2, (e) Rate performance, (f) Performance of assembled symmetric supercapacitor[91]
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