The development of optical films with high transparency,high thermal resistance and low birefringence remains a challenge in the flexible display industry.In this work,we designed and synthesized a series of fluorinat...The development of optical films with high transparency,high thermal resistance and low birefringence remains a challenge in the flexible display industry.In this work,we designed and synthesized a series of fluorinated colorless polyimides(CPIs)materials using 2,5-substituted m-phenylenediamine diamine monomers and 1,2,4,5-cyclohexanetetracarboxylic dianhydride(CHDA).We systematically studied the effects of fluorinated group substitutions on the thermal,mechanical,optical and dielectric properties of CPI films.The introduction of alicyclic CHDA dianhydride affords high transparency and low yellowness,while the 2,5-substituted m-phenylenediamine diamines offer the CPIs with quite low birefringence as well as high glass transition temperatures.A particular CHDA/o3FBDA film with simple chemical structure stands out,exhibiting well-balanced overall properties.展开更多
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supported by the Natural Science Foundation of Guangdong Province(No.2022A1515010125)the Key-Area Research and Development Program of Guangdong Province(No.2020B010182002)+5 种基金the Guangdong Basic and Applied Basic Research Foundation(No.2022A1515110543)the R&D Program of Guangzhou(No.2023A04J1577)the Major Program of National Natural Science Foundation of China(No.51890871)the Recruitment Program of Guangdong(No.2016ZT06C322)the 111 Project(No.B18023)Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application at Soochow University.
文摘The development of optical films with high transparency,high thermal resistance and low birefringence remains a challenge in the flexible display industry.In this work,we designed and synthesized a series of fluorinated colorless polyimides(CPIs)materials using 2,5-substituted m-phenylenediamine diamine monomers and 1,2,4,5-cyclohexanetetracarboxylic dianhydride(CHDA).We systematically studied the effects of fluorinated group substitutions on the thermal,mechanical,optical and dielectric properties of CPI films.The introduction of alicyclic CHDA dianhydride affords high transparency and low yellowness,while the 2,5-substituted m-phenylenediamine diamines offer the CPIs with quite low birefringence as well as high glass transition temperatures.A particular CHDA/o3FBDA film with simple chemical structure stands out,exhibiting well-balanced overall properties.
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.
