Thermal Expansion Behavior of Amide-containing Polyimide Films with Ultralow Thermal Expansion Coefficient †

doi:10.7503/cjcu20190563

Abstract

Abstract:

A series of amide-containing polyimide i. e. poly(amide-imide) films was prepared from biphenyl tetracarboxylic dianhydride and three diamines comprising diamide groups via two-step thermal imidization method. The effect of amide structure and different substituents on mechanical properties, water absorption, thermal properties and thermal expansion behavior of poly(amide-imide) films were investigated. The results showed that these films exhibited ultrahigh tensile strength up to 280.5 MPa and excellen theat resistance with T_g above 389 ℃. Moreover, these films showed ultralow thermal expansion coefficient(CTE) from -3.05 to -1.74 ppm/℃ in the wide temperature range of 30—300 ℃. The correlation of their thermal expansion behavior with aggregation structures including molecular chain interactions, orientation and packing was systematically studied. It was found that the molecular chains of poly(amide-imide)s were highly oriented along the in-plane direction while densely packed in the out-of-plane direction, because of the hydrogen bonding interactions between amide structures and the rigid linear backbone. That was the main reason for the thermal contraction of films and contributed to their outstanding dimensional stabilities. The aggregation structures of poly(amide-imide)s could be further affected by the substituents in the backbones with different volume and steric effect, resulting in the regulation of CTE values close to zero. It provids a new design thought for the heat-resistant polymer substrates with ultralow CTE for optoelectronic application.

Key words: Polyimide, Hydrogen bonding interaction, Aggregation structure, Thermal expansion behavior

CLC Number:

O631

TrendMD:

BAI Lan, ZHAI Lei, WANG Changou, HE Minhui, MO Song, FAN Lin. Thermal Expansion Behavior of Amide-containing Polyimide Films with Ultralow Thermal Expansion Coefficient ^†[J]. Chem. J. Chinese Universities, 2020, 41(4): 795.

Figures/Tables 11

Scheme 1 Synthetic routes of PAI-1, PAI-2 and PAI-3 APTA and PAI-1(s-BPDA/APTA): R=H; AFPTA and PAI-2(s-BPDA/AFPTA): R=F; AMPTA and PAI-3(s-BPDA/AMPTA): R=CH3

Fig.1 ATR-FTIR spectra of PAI-1(a), PAI-2(b) and PAI-3(c)

Fig.2 Water absorption, water contact angle and amide content of PAI-1, PAI-2 and PAI-3

Film	Tensile strength/MPa	Modulus/GPa	Elongation at break(%)
PAI-1	280.5±9.9	9.3±0.1	8.6±1.1
PAI-2	242.1±4.0	10.2±0.2	5.2±0.2
PAI-3	244.6±19.5	11.6±0.3	2.7±0.4

Fig.3 DMA(A) and TGA(B) curves of PAI-1, PAI-2 and PAI-3 films

Film	T_g/℃	T_d/℃	T_5%/℃	R_w(%)	CTE/(ppm·℃^-1)		[(ΔL-L₀)/L₀](%)
Film	T_g/℃	T_d/℃	T_5%/℃	R_w(%)	30—300 ℃	30—350 ℃	30—300 ℃	30—350 ℃
PAI-1	406	530	534	58.4	-3.05	-3.93	-0.082	-0.12
PAI-2	389	486	488	63.3	-2.62	-4.96	-0.071	0.17
PAI-3	409	499	510	61.3	-1.74	-5.31	-0.047	-0.16

Fig.4 TMA curves of PAI-1, PAI-2 and PAI-3 films

Film	n_TE	n_TM	n_av	Δn	d-spacing/nm	d(ch-pack)/nm
PAI-1	1.8542	1.6241	1.7808	0.2301	0.4312	0.4939
PAI-2	1.8471	1.6195	1.7713	0.2276	0.4323	0.4996
PAI-3	1.8291	1.6051	1.7544	0.2238	0.5092	0.5011
Ref-PI	1.7451	1.6682	1.7199	0.0769	0.4908	0.4937

Fig.5 Effects of birefringence(a) and averagere fractive(b) on the CTE of PAI-1, PAI-2 and PAI-3

Fig.6 Reflection(A) and transmission(B) WAXD patterns of PAI-1, PAI-2 and PAI-3 films

Fig.7 Effects of d-spacing and d(ch-pack) on the CTE of PAI-1, PAI-2 and PAI-3 films

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