Rational design of graphene/polymer composites with excellent electromagnetic interference shielding effectiveness and high thermal conductivity: a mini review

doi:10.1016/j.jmst.2021.10.052

Abstract

Abstract:

The integration and miniaturization of chips lead to inevitable overheating and increasing electromagnetic interference (EMI) problems, which threaten the performance, stability, and lifetime of electronic components. Therefore, it is important to improve the heat dissipation and EMI shielding performance in device packaging for the steady operation of electronic products. In recent years, due to its intrinsic superior thermal conductivity, proper electrical conductivity, light-weight, and structural adjustability, graphene has been widely used as high thermal and conductive fillers incorporated in the polymer matrix to improve the thermal conductivity and electrical conductivity of composites. This review concludes the recent development of graphene/polymer composites by using graphene as fillers to improve the thermal conductivity and EMI shielding effectiveness (EMI SE). The structure of graphene embedded in the composites varies from zero-dimension (0D), one-dimension (1D) to two-dimensions (2D). Moreover, highly thermally and electrically conductive fillers with different dimensions were also modified on the graphene to improve the composite performance. Finally, this review also makes prospects for the development trend of graphene/polymer composites with high thermal conductivity and EMI SE in the future.

Key words: Graphene/polymer composites, Structural design, Electromagnetic interference shielding, Thermal conductivity

Xue Tan, Qilong Yuan, Mengting Qiu, Jinhong Yu, Nan Jiang, Cheng-Te Lin, Wen Dai. Rational design of graphene/polymer composites with excellent electromagnetic interference shielding effectiveness and high thermal conductivity: a mini review[J]. J. Mater. Sci. Technol., 2022, 117: 238-250.

Figures/Tables 14

Fig. 1. Application scenarios of EMI shielding materials and TIMs in the 5G communications: (a) EMI shielding materials used in the SiP platform of the RF module. Reproduced with permission [6]. Copyright 2019, IEEE. and (b) TIMs used in the ball grid array (BGA) electronics package of 5G chip. Reproduced with permission [12]. Copyright 2018, Taylor & Francis.

Fig. 3. (a) “Sea-island” in low fillers loading. (b) Thermal conduction paths in high fillers loading. (c) Percolation phenomenon. (d) Thermoelastic coefficient theory. Reproduced with permission [79]. Copyright 2020, Elsevier.

Table 1. Comparison of EMI shielding performance and thermal conductivity of the polymer matrix composites with different structures.

Materials	Filler loading	Thickness (mm)	Density (g cm^-3)	Frequency (GHz)	EMI SE (dB)	SE_R (dB)	SE_A (dB)	SSE (dB cm³ g^-1)	SE/t (dB cm^-1)	SSE/t (dB cm² g^-1)	TC (W m^-1 K^-1)	TCE (%)	Ref
Random Dispersion													Empty Cell
GNP/PEDOT:PSS	10 wt%	0.8	1.031	8.2 - 12.4	46	2	44	46	575	570	0.6	216	[65]
GNP/EPDM	8 wt%	0.3	/	8.2 - 12.4	32.4	8.5	23.9	/	1080	/	0.79	243	[86]
Graphene/epoxy	19.5 vol%	1	/	8 - 12.4	65	10	55	/	650	/	11.2	3973	[87]
GNP/PLA	15 wt%	1	/	10	40	0.4	39.6	/	400	/	1.72	406	[88]
EG/LLDPE	31.6 vol%	1.5	/	8.2	33.1	2.4	30.7	/	221	/	6.5	1525	[89]
Interconnected Structure
Graphite foam/PDMS	15.9 wt%	4.5	0.17	8.2 - 18	31	8	23	183	69	407	0.076	102	[90]
Carbon Aerogel@rGO/PDMS	3.05 wt%	3	/	8.2 - 12.4	51	7	44	/	170	/	0.65	225	[91]
GNP/rGO/epoxy	20.5 wt%	3	/	8.2 - 12.4	51	8	43	/	170	/	1.56	609	[27]
rGO/GNP/PDMS	18.1 wt%	4	1.1	8.2 - 12.4	94	7.5	86.5	86	235	214	3	1513	[92]
EG/LLDPE	24.89 vol%	2	1.27	8 - 12	52.4	11.7	40.7	41	262	206	19.6	5927	[19]
Graphene/PW	23 wt%	/	/	8.2 - 12.4	48.2	15.5	32.7	/	/	/	28.7	14250	[93]
Anisotropic Orientation
Graphene film	100 wt%	0.014	2.05	8.2 - 12.4	73.7	/	/	36	52643	25680	803.1 (//)	/	[94]
rGO film	100 wt%	0.015	/	1	20.2	5.55	14.65	/	13467	/	1390 (//)	/	[95]
GNP/nylon	11.8 wt%	0.18	/	8.2 - 12.4	58.1	6.6	51.5	/	3228	/	15.8 (//)	6220	[96]
GNP/POM	48 wt%	0.15	/	10	44.7	9.6	31.4	/	2733	/	4.24 (⊥)	1111	[33]
Graphene Hybrids Composites - 0D Hybrid
Graphene/Ni/PC/SAN	3 wt%	/	/	18	29.4	/	/	/	/	/	0.7	276	[97]
Graphene/Cu/CPU	0.87 vol%	2	/	0 - 9	28.9-55.6	/	/	/	145-565	/	0.103	348	[98]
rGO@Fe₃O₄/epoxy	8.97	2	/	8.2	13.45	8.84	4.61	/	67	/	1.213 (//)	507	[99]
Fe₃O₄/GF/PDMS	12 wt%	2	/	8.2 - 12.4	70.37	11.67	58.7	/	352	/	28.12 (//)	1302	[16]
Graphene Hybrids Composites - 1D Hybrid
Graphene/cellulose nanofiber	25 wt%	0.033	1.36	8.2 - 12.4	27.4	12.3	15.1	20.15	8303	6106	33.55 (//)	/	[100]
rGO/cellulose nanofiber	50 wt%	0.023	/	8.2 - 12.4	26.2	8.5	17.7	/	11391	/	7.3 (//)	469	[101]
GNP/cellulose	90 wt%	0.013	/	8.2 - 12.4	43	18.6	24.4	/	33077	/	240.5 (//)	149	[102]
EG/cellulose nanofiber/PEO	97 wt%	0.012	/	8.2 - 12.4	44	20	24	/	36667	/	302.3 (//)	/	[103]
Graphene/SiCnw/ PVDF	9.5 wt%	1.2	/	9.2	32.1	7.5	24..5	/	268	/	2.13	914	[104]
Graphene/Ni/PVDF	20 wt%	0.5	/	18 - 26.5	43.3	11.5	31.7	/	866	/	8.96 (//)	1199	[105]
Graphene Hybrids Composites - 2D Hybrid
Cu/graphene	100 wt%	0.0088	/	1 - 18	52	/	/	/	59091	/	1932.73 (//)	/	[106]
GO/BN/SEBS-g-MAH/PHDDT	35 wt%	0.235	/	8.2 - 12.4	37.92	5.91	32.01	/	1614	/	12.62 (//)	/	[107]
MXene/rGO/PMMA	2 vol%	2	/	8 - 12	51	9.5	41.5	/	255	/	2.83	1472	[108]

Table 1. Comparison of EMI shielding performance and thermal conductivity of the polymer matrix composites with different structures.

Materials	Filler loading	Thickness (mm)	Density (g cm^-3)	Frequency (GHz)	EMI SE (dB)	SE_R (dB)	SE_A (dB)	SSE (dB cm³ g^-1)	SE/t (dB cm^-1)	SSE/t (dB cm² g^-1)	TC (W m^-1 K^-1)	TCE (%)	Ref
Random Dispersion													Empty Cell
GNP/PEDOT:PSS	10 wt%	0.8	1.031	8.2 - 12.4	46	2	44	46	575	570	0.6	216	[65]
GNP/EPDM	8 wt%	0.3	/	8.2 - 12.4	32.4	8.5	23.9	/	1080	/	0.79	243	[86]
Graphene/epoxy	19.5 vol%	1	/	8 - 12.4	65	10	55	/	650	/	11.2	3973	[87]
GNP/PLA	15 wt%	1	/	10	40	0.4	39.6	/	400	/	1.72	406	[88]
EG/LLDPE	31.6 vol%	1.5	/	8.2	33.1	2.4	30.7	/	221	/	6.5	1525	[89]
Interconnected Structure
Graphite foam/PDMS	15.9 wt%	4.5	0.17	8.2 - 18	31	8	23	183	69	407	0.076	102	[90]
Carbon Aerogel@rGO/PDMS	3.05 wt%	3	/	8.2 - 12.4	51	7	44	/	170	/	0.65	225	[91]
GNP/rGO/epoxy	20.5 wt%	3	/	8.2 - 12.4	51	8	43	/	170	/	1.56	609	[27]
rGO/GNP/PDMS	18.1 wt%	4	1.1	8.2 - 12.4	94	7.5	86.5	86	235	214	3	1513	[92]
EG/LLDPE	24.89 vol%	2	1.27	8 - 12	52.4	11.7	40.7	41	262	206	19.6	5927	[19]
Graphene/PW	23 wt%	/	/	8.2 - 12.4	48.2	15.5	32.7	/	/	/	28.7	14250	[93]
Anisotropic Orientation
Graphene film	100 wt%	0.014	2.05	8.2 - 12.4	73.7	/	/	36	52643	25680	803.1 (//)	/	[94]
rGO film	100 wt%	0.015	/	1	20.2	5.55	14.65	/	13467	/	1390 (//)	/	[95]
GNP/nylon	11.8 wt%	0.18	/	8.2 - 12.4	58.1	6.6	51.5	/	3228	/	15.8 (//)	6220	[96]
GNP/POM	48 wt%	0.15	/	10	44.7	9.6	31.4	/	2733	/	4.24 (⊥)	1111	[33]
Graphene Hybrids Composites - 0D Hybrid
Graphene/Ni/PC/SAN	3 wt%	/	/	18	29.4	/	/	/	/	/	0.7	276	[97]
Graphene/Cu/CPU	0.87 vol%	2	/	0 - 9	28.9-55.6	/	/	/	145-565	/	0.103	348	[98]
rGO@Fe₃O₄/epoxy	8.97	2	/	8.2	13.45	8.84	4.61	/	67	/	1.213 (//)	507	[99]
Fe₃O₄/GF/PDMS	12 wt%	2	/	8.2 - 12.4	70.37	11.67	58.7	/	352	/	28.12 (//)	1302	[16]
Graphene Hybrids Composites - 1D Hybrid
Graphene/cellulose nanofiber	25 wt%	0.033	1.36	8.2 - 12.4	27.4	12.3	15.1	20.15	8303	6106	33.55 (//)	/	[100]
rGO/cellulose nanofiber	50 wt%	0.023	/	8.2 - 12.4	26.2	8.5	17.7	/	11391	/	7.3 (//)	469	[101]
GNP/cellulose	90 wt%	0.013	/	8.2 - 12.4	43	18.6	24.4	/	33077	/	240.5 (//)	149	[102]
EG/cellulose nanofiber/PEO	97 wt%	0.012	/	8.2 - 12.4	44	20	24	/	36667	/	302.3 (//)	/	[103]
Graphene/SiCnw/ PVDF	9.5 wt%	1.2	/	9.2	32.1	7.5	24..5	/	268	/	2.13	914	[104]
Graphene/Ni/PVDF	20 wt%	0.5	/	18 - 26.5	43.3	11.5	31.7	/	866	/	8.96 (//)	1199	[105]
Graphene Hybrids Composites - 2D Hybrid
Cu/graphene	100 wt%	0.0088	/	1 - 18	52	/	/	/	59091	/	1932.73 (//)	/	[106]
GO/BN/SEBS-g-MAH/PHDDT	35 wt%	0.235	/	8.2 - 12.4	37.92	5.91	32.01	/	1614	/	12.62 (//)	/	[107]
MXene/rGO/PMMA	2 vol%	2	/	8 - 12	51	9.5	41.5	/	255	/	2.83	1472	[108]

Fig. 4. Schematic illustration of the fabrication process of GNPs/EPDM nanocomposites through mixing and compression molding process. Reproduced with permission [86]. Copyright 2019, World Scientific.

Fig. 5. (a) Bulk in-plane electrical conductivity of the graphene/epoxy composites versus FLG filler loading, the insert indicates the fabrication process of the graphene/epoxy composites. (b) Average reflection (red circles), absorption (blue triangles), and total EMI shielding (green squares) of composites over the entire X-band frequency range as a function of graphene loading. (c) Thermal conductivity of the composites as a function of graphene loading fraction at room temperature. (d) Total EMI SE of the epoxy with 17.1 vol% of graphene fillers as a function of temperature in the X-band frequency range. (e) The color map of the total EMI SE of the composites with 17.1 vol% of graphene fillers as a function of frequency in the temperature range from 303 K to 523 K. (f) Thermal conductivity of three composites with different graphene loading as a function of temperature. Reproduced with permission [87]. Copyright 2020, Wiley.

Fig. 6. (a) Schematic illustration of the fabrication procedure for CCA@rGO/PDMS EMI shielding composites. (b) SEM of CCA. (c) EMI SEA and SER of the CCA@rGO/PDMS EMI shielding composites. (d) Schematic illustration of EMI shielding mechanism. Reproduced with permission [91]. Copyright 2021, Springer Nature.

Fig. 8. (a) Schematic illustration of preparation process of graphene films. (b) The multi-layer model for graphene films composed of graphene laminates and (c) schematic illustration of electromagnetic waves reflection and transmission between two graphene laminates. Reproduced with permission [94]. Copyright 2019, Royal Society of Chemistry. (d) The schematic diagram of foldable and stretchable wrinkles. (e) The schematic diagram of electric or heat flow after adding GO or GNP. Reproduced with permission [109]. Copyright 2018, Elsevier.

Fig. 9. (a) Stepwise synthesis procedure for nickel decorated graphene sheets. (b) Thermal conductivity of various PC/SAN blends. (c) Total shielding effectiveness as a function of frequency for PC/SAN blends in X and Ku-band. Reproduced with permission [97]. Copyright 2015, Royal Society of Chemistry.

Fig. 10. Schematic of the fabrication procedure of GF/h-Fe3O4/PDMS composites and its effect in thermal conductivity and EMI SE enhancement. Reproduced with permission [16]. Copyright 2020, Elsevier.

Fig. 11. (a) Schematic process of preparing alternating multilayered CNF@GNS films through vacuum-assisted filtration. (b)Thermal conductivities of CNF@GNS5 film with different GNS filler loading. (c) Schematic diagrams of thermal conduction in CNF@GNS films (bottom) compared to direct mixed CNF/GNS (top). (d) EMI SE performance at the X-band with different content of GNS in the composite film. (e) Schematic illustration of EMW transfer across alternant layered CNF@GNS films. Reproduced with permission [100]. Copyright 2020, Elsevier.

Fig. 12. (a) Schematic delineations of the fabrication of Ni-graphene films. Schematic illustrations of (b, c) EMI shielding and (d, e) heat transfer mechanisms of Ni-G and Ni@G-P films. Reproduced with permission [105]. Copyright 2020, Elsevier.

Fig. 13. (a) The preparation process of the ordered multilayer film. (b) The optical photograph of the multilayer film. (c) SEM image of the multilayer film. (d) Thermal and electrical conductive schematic of the ordered multilayer film. Reproduced with permission [107]. Copyright 2016, Elsevier.

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