Photocatalytic hydrogen peroxide(H_(2)O_(2))production offers a sustainable route to convert water and oxygen into H_(2)O_(2)using solar energy.However,achieving long-term stability in photocatalysts remains a critica...Photocatalytic hydrogen peroxide(H_(2)O_(2))production offers a sustainable route to convert water and oxygen into H_(2)O_(2)using solar energy.However,achieving long-term stability in photocatalysts remains a critical challenge due to mismatched kinetics between oxygen reduction(ORR)and water oxidation(WOR),which leads to hole accumulation and oxidative degradation.Here,we report a redox-mediated strategy to address this bottleneck by designing a hydroquinone-embedded covalent organic framework(Tz-QH-COF)that enables reversible hole buffering and kinetic balance.The hydroquinone(QH)units act as dynamic hole reservoirs,capturing excess holes during ORR and converting to benzoquinone(Q),which is regenerated to QH via WOR,thereby preventing oxidative decomposition.This reversible QH/Q cycle,directly visualized through in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy,ensures unmatched stability,achieving continuous H_(2)O_(2) production for 528 h(22 d)with an accumulated yield of 18.6 mmol L^(–1)—the highest reported duration for organic photocatalysts.Density functional theory calculations reveal that the QH units exhibit a strong oxygen adsorption energy and favorable two-electron ORR/WOR pathways with low energy barriers.The synergy between experimental and theoretical insights elucidates a redox-mediated charge-balance mechanism,advancing the design of robust photocatalysts for solar-driven H_(2)O_(2) synthesis.展开更多
The enhanced performance of a squaraine compound, with 2,4-bis[4-（N,N-diisobutylamino）-2,6-dihydroxyphenyl] squaraine as the donor and [6,6]-phenyl-C71-butyric acid methyl ester （PC71BM） as the acceptor, in soluti...The enhanced performance of a squaraine compound, with 2,4-bis[4-（N,N-diisobutylamino）-2,6-dihydroxyphenyl] squaraine as the donor and [6,6]-phenyl-C71-butyric acid methyl ester （PC71BM） as the acceptor, in solution-processed or- ganic photovoltaic devices is obtained by using UV-ozone-treated MoO3 as the hole-collecting buffer layer. The optimized thickness of the MoO3 layer is 8 nm, at which the device shows the best power conversion efficiency （PCE） among all devices, resulting from a balance of optical absorption and charge transport. After being treated by UV-ozone for 10 min, the transmittance of the MoO3 film is almost unchanged. Atomic force microscopy results show that the treated surface morphology is improved. A high PCE of 3.99% under AM 1.5 G illumination （100 mW/cm2） is obtained.展开更多
Inserting a hole-buffer layer is an effective way to enhance emission efficiency of electroluminescence devices. We have successfully synthesized a new hole-buffer material PSB composed of pyrene, Schiff base and trih...Inserting a hole-buffer layer is an effective way to enhance emission efficiency of electroluminescence devices. We have successfully synthesized a new hole-buffer material PSB composed of pyrene, Schiff base and trihydroxy tert-butyl groups by the Suzuki-coupling reaction. The HOMO and LUMO lev-els were -6.33 eV and -2.55 eV, respectively, as estimated from cyclic volt-ammograms. In addition, homogeneous films (rms roughness ~2 nm) were readily obtained by spin-coating process. Multilayer polymer light-emitting diodes, ITO/PEDOT:PSS/PSB/SY/LiF/Al, have been fabricated using PSB as hole-buffer layer (HBL). Inserting PSB as HBL significantly enhances the per-formance (maximum luminance: 26,439 cd/m2, maximum current efficiency: 7.03 cd/A), compared with the one without PSB (9802 cd/m2, 2.43 cd/A). It is also superior to the device with conventional BCP as hole-blocking layer (ITO/PEDOT:PSS/SY/BCP/LiF/Al: 15,496 cd/m2, 5.56 cd/A). Current results strongly indicate that the PSB is a potential hole-buffer material for electrolu-minescent devices.展开更多
This work presents the synthesis of a new hole-buffering material TAZS and its successful application in polymer light-emitting diodes to enhance device performance. The TAZS is composed of aromatic 1,2,4-triazolylcor...This work presents the synthesis of a new hole-buffering material TAZS and its successful application in polymer light-emitting diodes to enhance device performance. The TAZS is composed of aromatic 1,2,4-triazolylcore linked with three trihydroxy tert-butyl terminals via azomethine linkages. The TAZS forms ashomogeneous film deposited by spin-coating process. The HOMO and LUMO levels of TAZS are -5.23 eV and -2.40 eV, respectively, as estimated from cyclic voltammogram. The current density results of hole-only and electron-only devices confirm strong hole-buffering capability of TAZS layer. Multilayer PLEDs with different thickness of TAZS (ITO/PEDOT: PSS/TAZS (x nm)/SY/ETL/LiF/Al) have been successfully fabricated, using spin-coating process to deposit hole-injecting PEDOT: PSS, TAZS, and emissive SY layers. The PLED with 16 nm TAZS reveals the optimal device performance, with maximum luminance and maximum current efficiency of 19,046 cd/m2 and 4.08 cd/A, respectively, surpassing those without TAZS as HBL (8484 cd/m2, 2.13 cd/A). The hole-buffering characteristic of TAZS contributes greatly to improved charges’ recombination ratio and enhanced emission efficiency.展开更多
文摘Photocatalytic hydrogen peroxide(H_(2)O_(2))production offers a sustainable route to convert water and oxygen into H_(2)O_(2)using solar energy.However,achieving long-term stability in photocatalysts remains a critical challenge due to mismatched kinetics between oxygen reduction(ORR)and water oxidation(WOR),which leads to hole accumulation and oxidative degradation.Here,we report a redox-mediated strategy to address this bottleneck by designing a hydroquinone-embedded covalent organic framework(Tz-QH-COF)that enables reversible hole buffering and kinetic balance.The hydroquinone(QH)units act as dynamic hole reservoirs,capturing excess holes during ORR and converting to benzoquinone(Q),which is regenerated to QH via WOR,thereby preventing oxidative decomposition.This reversible QH/Q cycle,directly visualized through in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy,ensures unmatched stability,achieving continuous H_(2)O_(2) production for 528 h(22 d)with an accumulated yield of 18.6 mmol L^(–1)—the highest reported duration for organic photocatalysts.Density functional theory calculations reveal that the QH units exhibit a strong oxygen adsorption energy and favorable two-electron ORR/WOR pathways with low energy barriers.The synergy between experimental and theoretical insights elucidates a redox-mediated charge-balance mechanism,advancing the design of robust photocatalysts for solar-driven H_(2)O_(2) synthesis.
基金Project supported by the Program for New Century Excellent Talents in University of Ministry of Education of China(Grant No.NCET-10-0220)the Specialized Research Fund for the Doctoral Program of Higher Education of China(Grant No.20120009130005)the Fundamental Research Funds for the Central Universities of Ministry of Education of China(Grant No.2012JBZ001)
文摘The enhanced performance of a squaraine compound, with 2,4-bis[4-（N,N-diisobutylamino）-2,6-dihydroxyphenyl] squaraine as the donor and [6,6]-phenyl-C71-butyric acid methyl ester （PC71BM） as the acceptor, in solution-processed or- ganic photovoltaic devices is obtained by using UV-ozone-treated MoO3 as the hole-collecting buffer layer. The optimized thickness of the MoO3 layer is 8 nm, at which the device shows the best power conversion efficiency （PCE） among all devices, resulting from a balance of optical absorption and charge transport. After being treated by UV-ozone for 10 min, the transmittance of the MoO3 film is almost unchanged. Atomic force microscopy results show that the treated surface morphology is improved. A high PCE of 3.99% under AM 1.5 G illumination （100 mW/cm2） is obtained.
文摘Inserting a hole-buffer layer is an effective way to enhance emission efficiency of electroluminescence devices. We have successfully synthesized a new hole-buffer material PSB composed of pyrene, Schiff base and trihydroxy tert-butyl groups by the Suzuki-coupling reaction. The HOMO and LUMO lev-els were -6.33 eV and -2.55 eV, respectively, as estimated from cyclic volt-ammograms. In addition, homogeneous films (rms roughness ~2 nm) were readily obtained by spin-coating process. Multilayer polymer light-emitting diodes, ITO/PEDOT:PSS/PSB/SY/LiF/Al, have been fabricated using PSB as hole-buffer layer (HBL). Inserting PSB as HBL significantly enhances the per-formance (maximum luminance: 26,439 cd/m2, maximum current efficiency: 7.03 cd/A), compared with the one without PSB (9802 cd/m2, 2.43 cd/A). It is also superior to the device with conventional BCP as hole-blocking layer (ITO/PEDOT:PSS/SY/BCP/LiF/Al: 15,496 cd/m2, 5.56 cd/A). Current results strongly indicate that the PSB is a potential hole-buffer material for electrolu-minescent devices.
文摘This work presents the synthesis of a new hole-buffering material TAZS and its successful application in polymer light-emitting diodes to enhance device performance. The TAZS is composed of aromatic 1,2,4-triazolylcore linked with three trihydroxy tert-butyl terminals via azomethine linkages. The TAZS forms ashomogeneous film deposited by spin-coating process. The HOMO and LUMO levels of TAZS are -5.23 eV and -2.40 eV, respectively, as estimated from cyclic voltammogram. The current density results of hole-only and electron-only devices confirm strong hole-buffering capability of TAZS layer. Multilayer PLEDs with different thickness of TAZS (ITO/PEDOT: PSS/TAZS (x nm)/SY/ETL/LiF/Al) have been successfully fabricated, using spin-coating process to deposit hole-injecting PEDOT: PSS, TAZS, and emissive SY layers. The PLED with 16 nm TAZS reveals the optimal device performance, with maximum luminance and maximum current efficiency of 19,046 cd/m2 and 4.08 cd/A, respectively, surpassing those without TAZS as HBL (8484 cd/m2, 2.13 cd/A). The hole-buffering characteristic of TAZS contributes greatly to improved charges’ recombination ratio and enhanced emission efficiency.
