Even though various nickel-nitrogen-carbon(Ni-N-C)combinations are prospective low-cost catalysts for the CO_(2)electroreduction reaction(CO_(2)RR),which is one avenue for attaining carbon neutrality,the detailed role...Even though various nickel-nitrogen-carbon(Ni-N-C)combinations are prospective low-cost catalysts for the CO_(2)electroreduction reaction(CO_(2)RR),which is one avenue for attaining carbon neutrality,the detailed role of different N species has hardly been investigated.Here,we report a hollow porous N-doped carbon nanofiber with NiNX-pyridinic N active species(denoted as h-Ni-N-C)developed using a facile electrospinning and SiO_(2)space-confined pyrolysis strategy.The NiNX-pyridinic N species are facilely generated during the pyrolysis process,giving rise to enhanced activity and selectivity for the CO_(2)RR.The optimized h-Ni-N-C exhibits a high CO Faradaic efficiency of 91.3%and a large current density of−15.1 mA cm^(−2)at−0.75 V versus reversible hydrogen electrode in an H-cell.Density functional theory(DFT)results show that NiN4-pyridinic N species demonstrate a lower free energy for the catalyst's rate-determining step than isolated NiN4 and pyridinic N species,without affecting the desorption of CO∗intermediate.展开更多
基金This work was financially supported by National Key Research and Development Program of China(2018YFB1502503).
文摘Even though various nickel-nitrogen-carbon(Ni-N-C)combinations are prospective low-cost catalysts for the CO_(2)electroreduction reaction(CO_(2)RR),which is one avenue for attaining carbon neutrality,the detailed role of different N species has hardly been investigated.Here,we report a hollow porous N-doped carbon nanofiber with NiNX-pyridinic N active species(denoted as h-Ni-N-C)developed using a facile electrospinning and SiO_(2)space-confined pyrolysis strategy.The NiNX-pyridinic N species are facilely generated during the pyrolysis process,giving rise to enhanced activity and selectivity for the CO_(2)RR.The optimized h-Ni-N-C exhibits a high CO Faradaic efficiency of 91.3%and a large current density of−15.1 mA cm^(−2)at−0.75 V versus reversible hydrogen electrode in an H-cell.Density functional theory(DFT)results show that NiN4-pyridinic N species demonstrate a lower free energy for the catalyst's rate-determining step than isolated NiN4 and pyridinic N species,without affecting the desorption of CO∗intermediate.
