Abstract
Developing low-cost,efficient,and stable non-precious-metal electrocatalysts with controlled crystal structure,morphology and compositions are highly desirable for hydrogen and oxygen evolution reactions.Herein,a series of phosphorus-doped Fe7S8 nanowires integrated within carbon (P-Fe7S8@C) are rationally synthesized via a one-step phosphorization of one-dimensional (1D) Fe-based organicinorganic nanowires.The as-obtained P-Fe7S8@C catalysts with modified electronic configurations present typical porous structure,providing plentiful active sites for rapid reaction kinetics.Density functional calculations demonstrate that the doping Fe7S8 with P can effectively enhance the electron density of Fe7S8 around the Fermi level and weaken the Fe-H bonding,leading to the decrease of adsorption free energy barrier on active sites.As a result,the optimal catalyst of P-Fe7S8-600@C exhibits a relatively low overpotential of 136 mV for hydrogen evolution reaction (HER) to reach the current density of 10 mA/cm2,and a significantly low overpotential of 210 mV for oxygen evolution reaction (OER) at 20mA/cm2 in alkaline media.The work presented here may pave the way to design and synthesis of other prominent Fe-based catalysts for water splitting via electronic regulation.
基金项目
work was financially supported by the National Natural Science Foundation of China(21601120)
work was financially supported by the National Natural Science Foundation of China(21805181)
Science and Technology Commission of Shanghai Municipality(17ZR1410500)
Science and Technology Commission of Shanghai Municipality(19ZR1418100)
We also appreciate the High Performance Computing Center of Shanghai University,and Shanghai Engineering Research Center of Inte(19DZ2252600)
NETL
NSTL
万方数据