Supporting Information

Revealing the Interrelation between Hydrogen Bonds and Interfaces in Graphene/PVA

Composites towards Highly Electrical Conductivity

Lijun Yang, Wei Weng, Xiang Fei*, Liang Pan, Xinao Li, Wenting Xu, Zexu Hu, Meifang Zhu*

State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science

and Engineering, Donghua University, 2999 North Renmin Road, Shanghai 201620, China;

Author information：* Corresponding author.

E-mails: zhumf@dhu.edu.cn (Meifang Zhu).

xiangfei@dhu.edu.cn (Xiang Fei)

First author: yanglijun211322@163.com(Lijun Yang)

S1

Figure S1. SEM images of loosely bound blocks after pre-aggregation treated. (a,b) SRGO; (c,d) HRGO.

S2

Figure S2. The FT-IR spectrum of different filler content in the PVA matrix.

S3

Figure S3. The variable temperature infrared spectrum of PVA/HRGO.

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Figure S4. Variable temperature FT-IR spectrum of PVA.

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Table S1. The fitting results of various kinds of hydrogen bonds in PVA-SRGO nanocomposite.

Temperature(C)

Hydrogen bond typeWavenumber

(cm1 )Peak area

Relative strength (%)

Standard deviation

65

Cyclic OH Ⅰ 3214 43.50 26.7 0.20OH…ether O Ⅱ 3304 43.65 26.8 1.75

Self-associated OH Ⅲ 3408 74.08 45.5 3.21OH…π Ⅳ 3513 1.47 0.9 0.13

85

Cyclic OH Ⅰ 3216 41.76 26.4 0.10OH…ether O Ⅱ 3303 38.76 24.5 2.01

Self-associated OH Ⅲ 3408 76.07 48.1 1.57OH…π Ⅳ 3514 1.64 1.0 0.22

105

Cyclic OH Ⅰ 3219 38.89 25.3 2.45

OH…ether O Ⅱ 3302 30.79 20.0 2.02Self-associated OH Ⅲ 3409 81.57 53.0 3.30

OH…π Ⅳ 3514 2.69 1.8 0.62

Table S2. The fitting results of various kinds of hydrogen bonds in PVA-HRGO nanocomposite.

Temperature(C)

Hydrogen bond typeWavenumber

(cm1)Peak area

Relative strength (%)

Standard deviation

65

Cyclic OHOH…ther O

Self-associated OHOH…π

ⅠⅡⅢⅣ

3218 3304 3410 3512

59.3174.66113.322.73

23.729.945.31.1

0.431.263.051.01

85

Cyclic OHOH…ether O

Self-associated OHOH…π

ⅠⅡⅢⅣ

3220 3303 3410 3513

56.6565.17116.883.56

23.426.948.21.5

1.323.862.240.80

105

Cyclic OHOH…ether O

Self-associated OHOH…π

ⅠⅡⅢⅣ

3221 3299 3408 3511

54.7654.03122.173.82

23.323.052.01.6

2.163.982.740.95

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Table S3. Comparison on conductivity between this work and the graphene and rGO-containing nanocomposite.

Filler Matrix*Maximum Loading

(wt%)Maximum

conductivity (S m1)Ref.

rGO

PVDF 7 ~10 [S1]PS 6.4 ~1 [S2]

PVA 7.5 ~10 [S3]PVA 14 5.92 [S4]PVA 50 ~1 [S5]

Epoxy 14 ~1 [S6]Epoxy 3 0.9 [S7]

Chitosan 6 1.2 [S8]Epoxy 6.6 0.16 [S9]

Graphene

PET 2.4 0.074 [S10]

SBR 15 3.7 [S11]HDPE 18 0.1 [S12]PVDF 4 0.031 [S13]

PU 10 0.25 [S14]PMMA 5 3.11 [S15]

UHMWPE 40 9.09 [S16]Epoxy 2 0.01 [S17]

PU 40 0.18 [S18]

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* PET: polyethylene glycol terephthalatePS: polystyrene PVDF: poly(vinylidene fluoride) HDPE: high-density polyethylene UHMWPE: Ultrahigh molecular weight polyethylene.

PVA: poly (vinyl alcohol); PMMA: polymethyl methacrylate; PU: polyurethane;SBR: styrene butadiene rubber;

Figure S5. The relationship between drawing temperature and maximum drawing ratio and conductivity.

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