Supporting online materials for

Compressive, ultralight and fire-resistant lignin-modified

graphene aerogels as recyclable absorbents for oil and

organic solvents

Changzhou Chen, Fengfeng Li, Yanru Zhang, Bingxin Wang, Yongming Fan, Xiluan Wang* and Runcang Sun

Beijing Key Laboratory of Lignocellulosic Chemistry, Beijing Forestry University, Beijing, 100083, P. R. China.

*Corresponding author: Tel: +86-10-62336903; Fax: +86-10-62336903

E-mail address: wangxiluan@bjfu.edu.cn

Fig. S1. The AFM image and height of GO sheets in this work.

Fig. S2. The solubility of (a) lignin and (b) GO sheets in pure water, pure alcohol and

alcohol solution (60%).

Fig. S3. (a) The nitrogen adsorption and desorption isotherms in Brunauer-Emmett-

Teller (BET) measurement. The pore size distribution of LGA calculated by (b)

Barrett-Joyner-Halenda (BJH) method and (c) mercury intrusion porosimetry (MIP)

method.

Fig. S4. The SEM images of the composite aerogels obtained from different feeding

ratio of lignin and GO, (a) 0:1, (b) 0.4:1, (c) 0.8:1 and (d) 1.2:1.

Fig. S5. Optical image of water droplet on the surface of the GA in contact angle

measurement.

Fig. S6. Absorption capacities of the LGAs in absorbing toluene after several

compression and release cycles.

Fig. S7. The dimensions of LGA before (a) and after (b) carbonization.

Fig. S8. SEM images of LGA (a) before and (b) after oil recycling after 10 cycles.

Fig. S9. The absorption and squeezing processes of LGA for absorbing dodecane in

an reuse cycle.

Fig. S10. Absorption capacities of the LGAs in absorbing dodecane after 20

squeezing cycles.

Table S1. Physical properties of GA and LGA.

Samples Density

(mg cm −3)

C/O

ratio

Maximum stress at

70% strain ( Pa)

Contact

angle

Porosity

(%)

GA 8.2 6.52 379 108° 94.3

LGA 3.0 5.15 275 127° 95.4

Table S2. Comparison of various graphene-based absorbent materials.

Sorbents Absorbates Capacity (g

g −1)

Ref.

N-doped graphene

framework

oils and organic

solvents

200–600 15

graphene-carbon nanotube

aerogels

oils and organic

solvents

215–913 18

Polydopamine-functionalized

carbon nanotubes-graphene

aerogel

oils and organic

solvents

125–533 44

Pure spongy graphene oils and organic

solvents

20–86 S1

rGO coated polyurethane

sponges

oils and organic

solvents

80–160 S2

Cu nanoparticles modified

graphene-based aerogels

Oils 28–40 S3

Graphene-polyvinylidene

fluoride aerogels

oils and organic

solvents

20–70 S4

Poly(acrylic acid)-rGO

Aerogels

oils 105–150 S5

Graphene aerogels oils and organic

solvents

110–240 S6

Graphene-based sponges oils and organic

solvents

54–165 S7

Graphene- Nanoribbon

Aerogels

oils and organic

solvents

121–302 S8

Dopamine modified graphene

aerogels

oils and organic

solvents

134–283 S9

Carbon nanotubes-graphene

hybrid aerogel

oils and organic

solvents

100–322 S10

Graphene oxide/nanofiber

aerogel

oils and organic

solvents

230–734  S11

Table S3. Comparison of various biomass-based absorbent materials.

Sorbents Absorbates Capacity Ref.

(g g −1)Lignin-based xerogel Oils and organic

solvents

19–47 31

Lignin-based

polyurethane/graphene oxide

foam

Oils and organic

solvents

26–68 33

lignin-melamine sponge Oils and organic

solvents

98–218 30

Cellulose-based aerogels Oils and organic

solvents

58–101 46

Carbon microbelt Aerogel Oils and organic

solvents

56–188 20

Nanocellulose carbon aerogel Oils 56–88 47Kapok fiber Organic solvents 21–30 45

Lignin-modified graphene

aerogels (LGA)

Oils and organic

solvents

167–350 Present

studyCarbonated lignin-modified

graphene aerogels (C-LGA)

Oils and organic

solvents

254–522 Present

study

References[S1] H. Bi, X. Xie, K. Yin, Y. Zhou, S. Wan, L. He, F. Xu, F. Banhart, L. Sun, R.S. Ruoff,

Graphene: spongy graphene as a highly efficient and recyclable sorbent for oils and organic

solvents, Adv. Funct. Mater. 2012 (2012) 4401-4401.

[S2] Y. Liu, J. Ma, T. Wu, X. Wang, G. Huang, Y. Liu, H. Qiu, Y. Li, W. Wang, J. Gao, Cost-

effective reduced graphene oxide-coated polyurethane sponge as a highly efficient and

reusable oil-absorbent, ACS Appl. Mater. Inter. 5 (2013) 10018-10026.

[S3] T. Wu, M. Chen, L. Zhang, X. Xu, Y. Liu, J. Yan, W. Wang, J. Gao, Three-dimensional

graphene-based aerogels prepared by a self-assembly process and its excellent catalytic and

absorbing performance, J. Mater. Chem. A 1 (2013) 7612-7621.

[S4] R. Li, C. Chen, J. Li, L. Xu, G. Xiao, D. Yan, A facile approach to superhydrophobic and

superoleophilic graphene/polymer aerogels, J. Mater. Chem. A 2 (2014) 3057-3064.

[S5] H. Ha, K. Shanmuganathan, C.J. Ellison, Mechanically Stable Thermally Crosslinked

Poly(acrylic acid)/Reduced Graphene Oxide Aerogels, ACS Appl. Mater. Inter. 7 (2015)

6220–6229.

[S6] F. Wang, Y. Wang, W. Zhan, S. Yu, W. Zhong, G. Sui, X. Yang, Facile synthesis of ultra-

light graphene aerogels with super absorption capability for organic solvents and strain-

sensitive electrical conductivity, Chem. Eng. J. 320 (2017) 539–548.

[S7] D.D. Nguyen, N.H. Tai, S.B. Lee, W.S. Kuo, Superhydrophobic and superoleophilic

properties of graphene-based sponges fabricated using a facile dip coating method, Energ.

Environ. Sci. 5 (2012) 7908-7912.

[S8] L. Chen, R. Du, J. Zhang, T. Yi, Density Controlled Oil Uptake and Beyond: From

Carbon Nanotube to Graphene Nanoribbon Aerogels, J. Mater. Chem. A 3 (2015) 20547-

20553.

[S9] L. Li, B. Li, J. Zhang, Dopamine-mediated fabrication of ultralight graphene aerogels

with low volume shrinkage, J. Mater. Chem. A 4 (2015) 512-518.

[S10] C. Wang, S. Yang, Q. Ma, X. Jia, P.C. Ma, Preparation of carbon nanotubes/graphene

hybrid aerogel and its application for the adsorption of organic compounds, Carbon 118

(2017) 765–771.

[S11] J. Xiao, W. Lv, Y. Song, Q. Zheng, Graphene/Nanofiber Aerogels: Performance

Regulation towards Multiple Applications in Dye Adsorption and Oil/water Separation,

Chem. Eng. J. 388 (2018) 202–210.