The development of high-performance transparent substrates is critical for next-generation flexible electronic devices.Herein,we designed two novel meta-substituted diamines incorporating trifluoromethyl(―CF_(3))and ...The development of high-performance transparent substrates is critical for next-generation flexible electronic devices.Herein,we designed two novel meta-substituted diamines incorporating trifluoromethyl(―CF_(3))and methyl(―CH_(3))groups to synthesize colorless copolyimide(CPI)films via copolymerization with 4,4′-(hexafluoroisopropylidene)diphthalic anhydride(6FDA)/3,3′,4,4′-biphenyltetracarboxylic dianhydride(BPDA).The combination of meta-substituted architecture and substituents enables the simultaneous attainment of an ultralow dielectric constant(D_k)and high transparency.The meta-substitution geometry and electronic effects of―CF_(3)/―CH_(3) effectively suppressed charge-transfer complex(CTC)formation,expanded fractional free volume(FFV),and restricted π-electron conjugation,as validated by DFT calculations and wide-angle X-ray diffraction(WAXD)analysis.The optimized CPI film(PIA_(1)-6FDA/BPDA(10/0))achieved outstanding transmittance(T_(450)=88.15%),ultralow dielectric constant(D_(k)=2.08 at 1 k Hz),and minimal dielectric loss(D_(f)=0.0012),while maintaining robust thermal stability(T_(d5%)>523℃)and mechanical strength(σ=87.5 MPa).This work establishes a molecular engineering strategy to concurrently enhance the optical and dielectric properties,positioning meta-substituted CPIs as promising candidates for transparent flexible devices.展开更多
基金financially supported by the National Key R&D Program of China(No.2023YFB3812400)the National Natural Science Foundation of China(No.51890871)the GJYC Program of Guangzhou(No.2024D02J0004)。
文摘The development of high-performance transparent substrates is critical for next-generation flexible electronic devices.Herein,we designed two novel meta-substituted diamines incorporating trifluoromethyl(―CF_(3))and methyl(―CH_(3))groups to synthesize colorless copolyimide(CPI)films via copolymerization with 4,4′-(hexafluoroisopropylidene)diphthalic anhydride(6FDA)/3,3′,4,4′-biphenyltetracarboxylic dianhydride(BPDA).The combination of meta-substituted architecture and substituents enables the simultaneous attainment of an ultralow dielectric constant(D_k)and high transparency.The meta-substitution geometry and electronic effects of―CF_(3)/―CH_(3) effectively suppressed charge-transfer complex(CTC)formation,expanded fractional free volume(FFV),and restricted π-electron conjugation,as validated by DFT calculations and wide-angle X-ray diffraction(WAXD)analysis.The optimized CPI film(PIA_(1)-6FDA/BPDA(10/0))achieved outstanding transmittance(T_(450)=88.15%),ultralow dielectric constant(D_(k)=2.08 at 1 k Hz),and minimal dielectric loss(D_(f)=0.0012),while maintaining robust thermal stability(T_(d5%)>523℃)and mechanical strength(σ=87.5 MPa).This work establishes a molecular engineering strategy to concurrently enhance the optical and dielectric properties,positioning meta-substituted CPIs as promising candidates for transparent flexible devices.
