

FOLLOWUS
a.Guangdong University of Technology (GDUT), Guangzhou 510006, China
b.Huimai Materials Technology (Guangdong) Co., Ltd., Foshan 528200, China
c.Shenzhen Customs Industrial Product Inspection Technology Center, Shenzhen 518026, China
ydliu@gdut.edu.cn (Y.D.L.)
cuitt@gdut.edu.cn (T.T.C.)
ygmin@gdut.edu.cn (Y.G.M.)
Received:07 April 2022,
Revised:2022-5-30,
Accepted:07 June 2022,
Online First:06 September 2022,
Published:01 February 2023
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Tan, W. Y.; Jian, L. F.; Chen, W. P.; Zhang, Y, W.; Lu, X. C.; Huang, W. J.; Zhang, J. S.; Wu, J. W.; Feng, J. L.; Liu, Y. D.; Cui, T. T.; Min, Y. G. A facile strategy for intrinsic low-Dk and low-Df polyimides enabled by spirobifluorene groups. Chinese J. Polym. Sci. 2023, 41, 288–296 DOI: 10.1007/s10118-022-2824-z.
Wan-Yi Tan, Ling-Feng Jian, Wei-Peng Chen, et al. A Facile Strategy for Intrinsic Low-
Tan, W. Y.; Jian, L. F.; Chen, W. P.; Zhang, Y, W.; Lu, X. C.; Huang, W. J.; Zhang, J. S.; Wu, J. W.; Feng, J. L.; Liu, Y. D.; Cui, T. T.; Min, Y. G. A facile strategy for intrinsic low-Dk and low-Df polyimides enabled by spirobifluorene groups. Chinese J. Polym. Sci. 2023, 41, 288–296 DOI: 10.1007/s10118-022-2824-z. DOI:
Wan-Yi Tan, Ling-Feng Jian, Wei-Peng Chen, et al. A Facile Strategy for Intrinsic Low-
A facile and effective strategy to afford low
D
k
/
D
f
MPIs with less fluoric groups and nonporous structure
through incorporating rigid and large sterically hindered spirobifluorene groups into the main chain.
Modified polyimides (MPIs) show great potential towards 5G communication applications
due to its excellent thermal stability
mechanical property and chemical stability as compared to most of polymers. Introducing fluoride groups or porous structure is favorable to ultra-low dielectric constant (
D
k
) and dielectric loss (
D
f
). However
the cost of the fluorinated MPIs is high and their synthetic processes are complicated
and porous MPIs suffer poor mechanical properties. Also
increasing the fraction of free volume is a very effective way to lower
D
k
through introducing more ultra-low-
D
k
air component. However
most of this kind of MPIs lag far behind the fluorinated MPIs and the porous MPIs in terms of ultra-low
D
f
hindering the application of MPIs in high-speed communication devices. Thus
it is highly desirable to develop intrinsic ultra-low-
D
k
/
D
f
MPIs at high frequency with less fluoric groups and nonporous structure. Herein
we introduce a facile and effective strategy to lower
D
k
and
D
f
through introducing rigid and large sterically hindered aromatic groups into MPIs. On the one hand
their large steric hindrance effect leads to low
D
k
by increasing intrinsic free volume. On the other hand
the resulting highly stiff polymer chain and strong intermolecular interaction are favorable to reduce
D
f
by inhibiting dipole orientations. Based on this strategy
the spirobifluorene groups are preferred. The as-prepared MPIs show excellent dielectric performance with low
D
k
of 2.74–2.76 and low
D
f
of 0.00599 at 10 GHz
to some extent
exceeding the multiple fluorinated MPI with
D
k
/
D
f
of 2.67/0.00663 at 10 GHz.
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