Modifying electrocatalysts nanostructures and tuning their electronic properties through defects-oriented synthetic strategies are:essential to improve the oxygen evolution reaction(OER)performance of electrocatalysts...Modifying electrocatalysts nanostructures and tuning their electronic properties through defects-oriented synthetic strategies are:essential to improve the oxygen evolution reaction(OER)performance of electrocatalysts.Current synthetic strategies about.electrocatalysts mainly target the single or double structural defects,while the researches about the synergistic effect of multiple'structural defects are rare.In this work,the ultrathin NiFe layered double hydroxide nanosheets with a holey structure,oxygen;vacancies and Ni^(3+)defects on nickel foam(NiFe-LDH-NSs/NF)are prepared by employing a simple and green H202-assisted etching 1 method.The synergistic effect ofthe above three defects leads to the exposure of.more active sites and significant improvement of:the intrinsic activity.The optimized catalyst exhibits an excellent OER performance with an extraordinarily low overpotential of 170 mV;at to mA·cm^(-2) and a small Tafel slope of 39.3 mV·dec^(-1) in 1 M KOH solution.Density functional theory calculations reveal this OER;performance arises from pseudo re-oxidized metal-stable Ni^(3+)near oxygen vacancies(O_(vac)),which suppresses 3d-e_(g) of Ni-site and!elevates d-band center towards the competitively low electron-transferbarrier.This work provides a new insight to fabricate advanced electrocatalysts for renewable energy conversion technologies.展开更多
基金supports from the National Natural Science Foundation of China(Nos.21531006 and 21773163)the State Key Laboratory of Organometallic Chemistry of Shanghai Institute of Organic Chemistry(No.KF2021005)Collaborative Innovation Center of Suzhou Nano Science and Technology,the“Priority Academic Program Development”of Jiangsu Higher Education Institutions,and the Project of Scientific and Technologic Infrastructure of Suzhou(No.SZS201905).
文摘Modifying electrocatalysts nanostructures and tuning their electronic properties through defects-oriented synthetic strategies are:essential to improve the oxygen evolution reaction(OER)performance of electrocatalysts.Current synthetic strategies about.electrocatalysts mainly target the single or double structural defects,while the researches about the synergistic effect of multiple'structural defects are rare.In this work,the ultrathin NiFe layered double hydroxide nanosheets with a holey structure,oxygen;vacancies and Ni^(3+)defects on nickel foam(NiFe-LDH-NSs/NF)are prepared by employing a simple and green H202-assisted etching 1 method.The synergistic effect ofthe above three defects leads to the exposure of.more active sites and significant improvement of:the intrinsic activity.The optimized catalyst exhibits an excellent OER performance with an extraordinarily low overpotential of 170 mV;at to mA·cm^(-2) and a small Tafel slope of 39.3 mV·dec^(-1) in 1 M KOH solution.Density functional theory calculations reveal this OER;performance arises from pseudo re-oxidized metal-stable Ni^(3+)near oxygen vacancies(O_(vac)),which suppresses 3d-e_(g) of Ni-site and!elevates d-band center towards the competitively low electron-transferbarrier.This work provides a new insight to fabricate advanced electrocatalysts for renewable energy conversion technologies.
