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
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.
