Rational design of defected carbons adjacent to nitrogen(N)dopants is a fascinating but challenging approach for enhancing the catalytic performance of N-doped carbon.Meanwhile,the combined effect of heteroatom doping...Rational design of defected carbons adjacent to nitrogen(N)dopants is a fascinating but challenging approach for enhancing the catalytic performance of N-doped carbon.Meanwhile,the combined effect of heteroatom doping and defect engineering can efficiently increase the oxygen reduction reaction(ORR)ability of inactive carbons through charge redistribution.Herein,we report that an enhanced built-in electric field caused by the combined effect of N-doping and carbon defects in the twodimensional(2D)mesoporous N-doped carbon nano flakes(NCNF)is a promising technique for improving ORR performance.As a result,the NCNF exhibits more promising ORR activity than Pt/C and similar performance with reported robust catalysts.Comprehensive experimental and theoretical investigations suggest that topologically defected carbon adjacent to the graphitic valley nitrogen is a real active site,rendering optimal energy for the adsorption of ORR intermediates and lowering the total energy barrier for ORR.Also,NCNF-based Zn-air batteries exhibited an excellent power density and specific capacity of~121.10 mW cm^(-2)and~679.86 mA h g_(Zn)^(-1),respectively.This study not only offers new insights into defected carbons with graphitic valley N for ORR but also proposes novel catalyst design principles and provides a solid grasp of the built-in electric field effect on the ORR performance of defective catalysts.展开更多
Perovskite and organic solar cells usually require electron-transport interlayers to efficiently transport electrons from the photoactive layer to the metal electrode.In general,pure organic or inorganic materials are...Perovskite and organic solar cells usually require electron-transport interlayers to efficiently transport electrons from the photoactive layer to the metal electrode.In general,pure organic or inorganic materials are applied into the interlayers,but organic–inorganic hybrid materials have been rarely reported for this application.In this work,we report using the first titanium-oxo cluster-based organic–inorganic hybrid as the interlayer material by introducing largeπ-conjugated benzo[ghi]perylenetriimides as an organic part via a simple ligand-exchange reaction.This new hybrid material showed excellent solubility,well-aligned energy levels,and excellent electron mobilities,enabling its great potential application as an interlayer in solar cells such as perovskite and organic solar cells,providing high power conversion efficiencies of>20%and 16%,respectively.Therefore,we claim that our present work introduces a new class of cluster-based organic–inorganic hybrid interlayer materials that exhibit promising application in organic electronics.展开更多
基金supported by the National Natural Science Foundation of China(22262010,22062005,22165005,U20A20128)Guangxi Science and Technology Fund for Distinguished HighTalent Introduction Program(AC22035091)Guangxi Science Fund for Distinguished Young Scholars(2019GXNSFFA245016)。
文摘Rational design of defected carbons adjacent to nitrogen(N)dopants is a fascinating but challenging approach for enhancing the catalytic performance of N-doped carbon.Meanwhile,the combined effect of heteroatom doping and defect engineering can efficiently increase the oxygen reduction reaction(ORR)ability of inactive carbons through charge redistribution.Herein,we report that an enhanced built-in electric field caused by the combined effect of N-doping and carbon defects in the twodimensional(2D)mesoporous N-doped carbon nano flakes(NCNF)is a promising technique for improving ORR performance.As a result,the NCNF exhibits more promising ORR activity than Pt/C and similar performance with reported robust catalysts.Comprehensive experimental and theoretical investigations suggest that topologically defected carbon adjacent to the graphitic valley nitrogen is a real active site,rendering optimal energy for the adsorption of ORR intermediates and lowering the total energy barrier for ORR.Also,NCNF-based Zn-air batteries exhibited an excellent power density and specific capacity of~121.10 mW cm^(-2)and~679.86 mA h g_(Zn)^(-1),respectively.This study not only offers new insights into defected carbons with graphitic valley N for ORR but also proposes novel catalyst design principles and provides a solid grasp of the built-in electric field effect on the ORR performance of defective catalysts.
基金supported by MOST(nos.2018YFA0208504 and 2017YFA0204702)NSFC(51773207,52073016,5197030531,and 21801213)of China+2 种基金The Fundamental Research Funds for the Central Universities further supported this work(no.XK1802-2)Open Project of State Key Laboratory of Supramolecular Structure and Materials(no.sklssm202043)Jiangxi Provincial Department of Science and Technology(nos.20192ACB20009,20192BBEL50026,20202ACBL213004,and 20203BBE53062).
文摘Perovskite and organic solar cells usually require electron-transport interlayers to efficiently transport electrons from the photoactive layer to the metal electrode.In general,pure organic or inorganic materials are applied into the interlayers,but organic–inorganic hybrid materials have been rarely reported for this application.In this work,we report using the first titanium-oxo cluster-based organic–inorganic hybrid as the interlayer material by introducing largeπ-conjugated benzo[ghi]perylenetriimides as an organic part via a simple ligand-exchange reaction.This new hybrid material showed excellent solubility,well-aligned energy levels,and excellent electron mobilities,enabling its great potential application as an interlayer in solar cells such as perovskite and organic solar cells,providing high power conversion efficiencies of>20%and 16%,respectively.Therefore,we claim that our present work introduces a new class of cluster-based organic–inorganic hybrid interlayer materials that exhibit promising application in organic electronics.
