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Inte
nsity
2θ (degree)
Si Si* Si*@PDA
Fig. S1 Enlarged XRD patterns of Si, Si* and Si*@PDA.
10 20 30 40 50 60 70 80 90
Inte
nsity
2θ (degree)
Si Si (N2)
100 200 300 400 500 600 700 800 90090
92
94
96
98
100
102
104
106
Wei
ght (
wt %
)
Temperature (oC)
Si Si* Si*@PDA Si (N2)
(a) (b)
Fig. S2 (a) TGA curves of Si, Si* and Si*@PDA under air and Si under nitrogen atmosphere. (b) XRD pattern of Si under air and nitrogen, respectively.
10 μm10 μm
a b
5 μm
network
Fig. S3 SEM images of fractured surface of (a) 25.5 vol% Si/epoxy, (b) 33.8 vol% Si/epoxy.
25 50 75 100 125 150 175 2000.00.10.20.30.40.50.60.70.80.91.01.11.21.31.41.5
The
rmal
Con
duct
ivity
(W/m
K)
Temperature (oC)
Neat epoxy 10 wt% Si*@PDA 20 wt% Si*@PDA 30 wt% Si*@PDA 40 wt% Si*@PDA 50 wt% Si*@PDA
Fig. S4 Thermal conductivity of Si*@PDA/composite as a function of test temperature.
Table S1 Thermal properties of pure epoxy and Si*@PDA/epoxy composites with various filler loading.
SampleWeight loss temperature ( )℃ Glass transition temperature ( )℃
T5% T10% Tmax Tg(DSC) ΔTg(DSC) Tg(DMA) ΔTg(DMA)
Pure Epoxy 330.8 357.2 399.7 130.1 - 130.5 -5.4 vol% Si*@PDA 363.0 375.8 405.2 139.1 9.0 143.4 12.911.4 vol% Si*@PDA 358.2 374.8 406.0 134.5 4.4 136.6 6.118.0 vol% Si*@PDA 357.8 373.8 406.3 133.1 3.0 132.8 2.325.5 vol% Si*@PDA 360.3 377.8 407.9 131.6 1.5 131.2 0.733.8 vol% Si*@PDA 359.3 376.5 406.8 130.7 0.6 130.9 0.4
100 200 300 400 500 600 700 8000
102030405060708090
100
Pure Epoxy 5.4 vol% Si*@PDA 11.4 vol% Si*@PDA 18.0 vol% Si*@PDA 25.5 vol% Si*@PDA 33.8 vol% Si*@PDA
Temperature (oC)
Wei
ght (
%)
Fig. S5 TGA curves of the Si*@PDA/epoxy composites with different filler content under nitrogen atmosphere.
80 90 100 110 120 130 140 150 160 170 180
Temperature (oC)
Pure Epoxy 10 wt% Si*@PDA/Epoxy 20 wt% Si*@PDA/Epoxy 30 wt% Si*@PDA/Epoxy 40 wt% Si*@PDA/Epoxy 50 wt% Si*@PDA/Epoxy
Heat
Flo
w (m
W)
Fig. S6 DSC curves of the Si*@PDA/epoxy composites with different filler content under nitrogen atmosphere.
20 40 60 80 100 120 140 160 180 200 220
0
500
1000
1500
2000
2500
3000
3500
4000
Stor
age
Mod
ulus
(MPa
)
Epoxy 10 wt% Si*@PDA/epoxy 20 wt% Si*@PDA/epoxy 30 wt% Si*@PDA/epoxy 40 wt% Si*@PDA/epoxy 50 wt% Si*@PDA/epoxy
Temperature (oC)80 90 100 110 120 130 140 150 160
-0.2
0.0
0.2
0.4
0.6
0.8
1.0
1.2
1.4
Tanδ
Pure Epoxy 5.4 vol% Si*@PDA 11.4 vol% Si*@PDA 18.0 vol% Si*@PDA 25.5 vol% Si*@PDA 33.8 vol% Si*@PDA
Temperature (oC)
(a) (b)
Fig. S7 DMA curves of the Si*@PDA/epoxy composites with different filler content.