Photocatalytic splitting of hydrogen sulfide(H2S) for hydrogen evolution is a promising method to solve the energy and environmental issues.In this work,S,N-codoped carbon dots(S,N-CDs)/graphitic carbon nitride(g-C3N4...Photocatalytic splitting of hydrogen sulfide(H2S) for hydrogen evolution is a promising method to solve the energy and environmental issues.In this work,S,N-codoped carbon dots(S,N-CDs)/graphitic carbon nitride(g-C3N4) nanosheet is synthesized by hydrothermal method as an efficient photocatalyst for the decomposition of H2S.In addition to the characterization of the morphology and structure,chemical state,optical and electrochemical performances of S,N-CDs/g-C3N4,hydrogen evolution tests show that the activity of g-C3N4 is improved by introducing S,N-CDs,and the enhancement depends strongly on the wavelength of incident light.The photocatalytic hydrogen production rate of S,N-CDs/g-C3N4 composite reaches 832 μmol g-1h-1, which is 38 times to that of g-C3N4 under irradiation at 460 nm.Density functional theory calculations and electron paramagnetic resonance as well as photoluminescence technologies have altogether authenticated that the unique wavelength-dependent photosensitization of S,N-CDs on g-C3N4;meanwhile,a good match between the energy level of S,N-CDs and g-C3N4 is pivotal for the effective photocatalytic activity.Our work has unveiled the detailed mechanism of the photocatalytic activity enhancement in S,N-CDs/g-C3N4 composite and showed its potential in photocatalytic splitting of H2S for hydrogen evolution.展开更多
Quantum dot light-emitting diodes(QD-LEDs)are considered as competitive candidate for next-generation displays or lightings.Recent advances in the synthesis of core/shell quantum dots(QDs)and tailoring procedures for ...Quantum dot light-emitting diodes(QD-LEDs)are considered as competitive candidate for next-generation displays or lightings.Recent advances in the synthesis of core/shell quantum dots(QDs)and tailoring procedures for achieving their high quantum yield have facilitated the emergence of high-performance QD-LEDs.Meanwhile,the charge-carrier dynamics in QD-LED devices,which constitutes the remaining core research area for further improvement of QD-LEDs,is,however,poorly understood yet.Here,we propose a charge transport model in which the charge-carrier dynamics in QD-LEDs are comprehensively described by computer simulations.The charge-carrier injection is modelled by the carrier-capturing process,while the effect of electric fields at their interfaces is considered.The simulated electro-optical characteristics of QD-LEDs,such as the luminance,current density and external quantum efficiency(EQE)curves with varying voltages,show excellent agreement with experiments.Therefore,our computational method proposed here provides a useful means for designing and optimising high-performance QD-LED devices.展开更多
基金financial support from the National Natural Science Foundation of China (U1862111 and 21702213)Cheung Kong Scholars Programme of China+3 种基金Chinese Academic of Science “light of west China” ProgramProvincial International Cooperation Project 2020YFH0118, Sichuan, ChinaOpen Fund (PLN201802 and 201928) of State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation (Southwest Petroleum University)Open Fund of State Key Laboratory of Industrial Vent Gas Reuse (SKLIVGR-SWPU-2020-05)。
文摘Photocatalytic splitting of hydrogen sulfide(H2S) for hydrogen evolution is a promising method to solve the energy and environmental issues.In this work,S,N-codoped carbon dots(S,N-CDs)/graphitic carbon nitride(g-C3N4) nanosheet is synthesized by hydrothermal method as an efficient photocatalyst for the decomposition of H2S.In addition to the characterization of the morphology and structure,chemical state,optical and electrochemical performances of S,N-CDs/g-C3N4,hydrogen evolution tests show that the activity of g-C3N4 is improved by introducing S,N-CDs,and the enhancement depends strongly on the wavelength of incident light.The photocatalytic hydrogen production rate of S,N-CDs/g-C3N4 composite reaches 832 μmol g-1h-1, which is 38 times to that of g-C3N4 under irradiation at 460 nm.Density functional theory calculations and electron paramagnetic resonance as well as photoluminescence technologies have altogether authenticated that the unique wavelength-dependent photosensitization of S,N-CDs on g-C3N4;meanwhile,a good match between the energy level of S,N-CDs and g-C3N4 is pivotal for the effective photocatalytic activity.Our work has unveiled the detailed mechanism of the photocatalytic activity enhancement in S,N-CDs/g-C3N4 composite and showed its potential in photocatalytic splitting of H2S for hydrogen evolution.
基金This research was supported by the European Union under H2020 grant agreement No 685758‘1D-NEON’by the Engineering and Physical Sciences Research Council(EPSRC)project EP/P027628/1‘Smart Flexible Quantum Dot Lighting’.
文摘Quantum dot light-emitting diodes(QD-LEDs)are considered as competitive candidate for next-generation displays or lightings.Recent advances in the synthesis of core/shell quantum dots(QDs)and tailoring procedures for achieving their high quantum yield have facilitated the emergence of high-performance QD-LEDs.Meanwhile,the charge-carrier dynamics in QD-LED devices,which constitutes the remaining core research area for further improvement of QD-LEDs,is,however,poorly understood yet.Here,we propose a charge transport model in which the charge-carrier dynamics in QD-LEDs are comprehensively described by computer simulations.The charge-carrier injection is modelled by the carrier-capturing process,while the effect of electric fields at their interfaces is considered.The simulated electro-optical characteristics of QD-LEDs,such as the luminance,current density and external quantum efficiency(EQE)curves with varying voltages,show excellent agreement with experiments.Therefore,our computational method proposed here provides a useful means for designing and optimising high-performance QD-LED devices.