Molecular electrocatalysts have demonstrated potential for the hydrogen evolution reaction(HER)due to their well-defined structures and high intrinsic activities.Achieving rapid production of hydrogen requires molecul...Molecular electrocatalysts have demonstrated potential for the hydrogen evolution reaction(HER)due to their well-defined structures and high intrinsic activities.Achieving rapid production of hydrogen requires molecular electrocatalysts to operate at high current densities,which still presents a challenge.In this work,we demonstrate that molecularly dispersed electrocatalysts of cobalt phthalocyanine anchored on carbon nanotubes(CoPc MDEs)are superior candidates due to the efficient charge transport between the substrate and the active site.The intrinsic activity can be enhanced by introducing functional groups on phthalocyanine.To facilitate mass transport,di(ethylene glycol)substituted CoPc molecules are further anchored on a threedimensional self-supported electrode(CoPc-DEG MDE@CC),enabling continuous operation for 25 h at−1000 mA/cm^(2)in 1.0 M KOH.Our study demonstrates the potential of molecular electrocatalysts for HER and emphasizes the importance of adjusting intrinsic activity,and charge and mass transport capacity for practical molecular electrocatalysts.展开更多
Charge manipulation is crucial in optoelectronic devices.The unoptimized interfacial charge injection/extraction in solution-processed bulkheterojunction(BHJ)organic photodetectors(OPDs)presents significant challenges...Charge manipulation is crucial in optoelectronic devices.The unoptimized interfacial charge injection/extraction in solution-processed bulkheterojunction(BHJ)organic photodetectors(OPDs)presents significant challenges in achieving high detectivity and fast response speed.Here,we first develop an approach for intrinsic charge manipulation induced by molecularly engineered donors to block electron injection and facilitate hole extraction between the indium tin oxide(ITO)transparent anode and the photoactive layer.By utilizing a polymer donor with 3,4-ethylenedioxythiophene(EDOT)as the conjugated side chain,a polymer-rich layer forms spontaneously on the ITO substrate due to the increased oxygen interactions between ITO and EDOT.This results in electron-blocking-layer(EBL)-free devices with lower dark current and noise without a reduction in responsivity compared to control devices.As a result,the EBL-free devices exhibit a peak specific detectivity of 2.36×10^(13) Jones at 950 nm and achieve a-3 dB bandwidth of 30 MHz under-1 V.Enhanced stability is also observed compared to the devices with poly(3,4-ethylenedioxythiophene)polystyrene sulfonate(PEDOT:PSS).This work demonstrates a new method to intrinsically manipulate charge injection in BHJ photoactive layers,enabling the fabrication of solution-processed EBL-free OPDs with high sensitivity,rapid response,and good stability.展开更多
基金supported by Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices(No.2019B121205001)Shenzhen fundamental research funding(Nos.JCYJ20220818100618039 and JCYJ20200109141405950)+1 种基金the National Natural Science Foundation of China(No.22075125)supported by the Center for Computational Science and Engineering(SUSTech).
文摘Molecular electrocatalysts have demonstrated potential for the hydrogen evolution reaction(HER)due to their well-defined structures and high intrinsic activities.Achieving rapid production of hydrogen requires molecular electrocatalysts to operate at high current densities,which still presents a challenge.In this work,we demonstrate that molecularly dispersed electrocatalysts of cobalt phthalocyanine anchored on carbon nanotubes(CoPc MDEs)are superior candidates due to the efficient charge transport between the substrate and the active site.The intrinsic activity can be enhanced by introducing functional groups on phthalocyanine.To facilitate mass transport,di(ethylene glycol)substituted CoPc molecules are further anchored on a threedimensional self-supported electrode(CoPc-DEG MDE@CC),enabling continuous operation for 25 h at−1000 mA/cm^(2)in 1.0 M KOH.Our study demonstrates the potential of molecular electrocatalysts for HER and emphasizes the importance of adjusting intrinsic activity,and charge and mass transport capacity for practical molecular electrocatalysts.
基金the Shenzhen Fundamental Research Funding(Key Program,No.JCYJ20200109141405950)Shenzhen Key Lab Funding(No.ZDSYS2015052915525382)+6 种基金the National Natural Science Foundation of China(No.51703092)the European Research Council for support under the European Union's Horizon 2020 Research and Innovation Program(Nos.742708 and 648901)support under Guangdong Provincial Natural Science Foundation General Project(No.2024A1515012318)Guangdong Basic and Applied Basic Research Foundation(No.2023A1515111140)Shenzhen government for support under the special appointed position-“Pengcheng Peacock Plan-C”The Chinese University of Hong Kong(Shenzhen)for support under The University Development Fund(No.UDF01003117)Special Funds for High-Level Universities-Talent Projects-“Presidential Young Fellow”(No.UF02003117).
文摘Charge manipulation is crucial in optoelectronic devices.The unoptimized interfacial charge injection/extraction in solution-processed bulkheterojunction(BHJ)organic photodetectors(OPDs)presents significant challenges in achieving high detectivity and fast response speed.Here,we first develop an approach for intrinsic charge manipulation induced by molecularly engineered donors to block electron injection and facilitate hole extraction between the indium tin oxide(ITO)transparent anode and the photoactive layer.By utilizing a polymer donor with 3,4-ethylenedioxythiophene(EDOT)as the conjugated side chain,a polymer-rich layer forms spontaneously on the ITO substrate due to the increased oxygen interactions between ITO and EDOT.This results in electron-blocking-layer(EBL)-free devices with lower dark current and noise without a reduction in responsivity compared to control devices.As a result,the EBL-free devices exhibit a peak specific detectivity of 2.36×10^(13) Jones at 950 nm and achieve a-3 dB bandwidth of 30 MHz under-1 V.Enhanced stability is also observed compared to the devices with poly(3,4-ethylenedioxythiophene)polystyrene sulfonate(PEDOT:PSS).This work demonstrates a new method to intrinsically manipulate charge injection in BHJ photoactive layers,enabling the fabrication of solution-processed EBL-free OPDs with high sensitivity,rapid response,and good stability.
