Rational design of non-noble electrocatalysts with high performance for oxygen evolution reaction(OER)still remains a challenge.In this study,a ZIF-derived electrocatalyst(Co@Fe-P)with a core-shell structure is design...Rational design of non-noble electrocatalysts with high performance for oxygen evolution reaction(OER)still remains a challenge.In this study,a ZIF-derived electrocatalyst(Co@Fe-P)with a core-shell structure is designed by using Co-compounds as the core and PO_(4)^(3-)decorated Fe-compounds as the shell.The inner Co-core and outer Fe-shell are connected through Co-O-Fe and Fe-O-P linkage.The Co@Fe-P electrocatalyst exhibits an enhanced performance for OER with a low overpotential(280 mV),low Tafel slope(41.9 mV dec^(-1))at 10 mA cm^(-2),and a 60-h durability.The electron transfer from the CoOOH-core to the FeOOH-shell is greatly facilitated,which improves the OER activity of Co@Fe-P kinetically.Theoretical calculations indicate that the interaction of Co-O-Fe and Fe-O-P in Co@Fe-P reduces the overlap between the O 2p and Fe 3d orbitals,which greatly facilitates the transformation from*OH to*O during the OER process via the adsorbate evolution mechanism(AEM)pathway.This finding provides insight for the design of efficient electrocatalysts for OER.展开更多
Due to larger atom utilization,unique electronic properties and unsaturated coordination,atomically dispersed non-precious metal catalysts with outstanding performances have received great attention in electrocatalysi...Due to larger atom utilization,unique electronic properties and unsaturated coordination,atomically dispersed non-precious metal catalysts with outstanding performances have received great attention in electrocatalysis.Considering the challenge of serious aggregation,rational synthesis of an atomic catalyst with good dispersion of atoms is paramount to the development of these catalysts.Herein,we report an enhanced confinement strategy to synthesize a catalyst comprised of atomically dispersed Fe supported on porous nitrogen-doped graphitic carbon from the novel and more cross-linkable Melamine-Glyoxal Resin.Densified isolated grid trapping,excessive melamine restricting,and nitrogen anchoring are strongly combined to ensure the final atomic-level dispersion of metal atoms.Experimental studies revealed enhanced kinetics of the obtained catalyst towards oxygen reduction reaction(ORR).This catalytic activity originates from the highly active surface with atomically dispersed iron sites as well as the multi-level three-dimensional structure with fast mass and electron transfer.The enhanced confinement strategy endows the resin-derived atomic catalyst with a great prospect to develop for commercialization in future.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.22372143 and 22208281)the Hebei Natural Science Foundation(Nos.B2023203001 and B2025203050)the Science Research Project of Hebei Education Department(BJK2024122)。
文摘Rational design of non-noble electrocatalysts with high performance for oxygen evolution reaction(OER)still remains a challenge.In this study,a ZIF-derived electrocatalyst(Co@Fe-P)with a core-shell structure is designed by using Co-compounds as the core and PO_(4)^(3-)decorated Fe-compounds as the shell.The inner Co-core and outer Fe-shell are connected through Co-O-Fe and Fe-O-P linkage.The Co@Fe-P electrocatalyst exhibits an enhanced performance for OER with a low overpotential(280 mV),low Tafel slope(41.9 mV dec^(-1))at 10 mA cm^(-2),and a 60-h durability.The electron transfer from the CoOOH-core to the FeOOH-shell is greatly facilitated,which improves the OER activity of Co@Fe-P kinetically.Theoretical calculations indicate that the interaction of Co-O-Fe and Fe-O-P in Co@Fe-P reduces the overlap between the O 2p and Fe 3d orbitals,which greatly facilitates the transformation from*OH to*O during the OER process via the adsorbate evolution mechanism(AEM)pathway.This finding provides insight for the design of efficient electrocatalysts for OER.
基金financially supported by the Hebei Province Natural Science Foundation Innovation Group Project(B2021203016)the National Natural Science Foundation of China(51674221 and 51704261)+1 种基金the Provincial Graduate Innovation Assistant Project of Yanshan University(023000309)partially supported by the ARC Future Fellowship(FT180100705)of Australia。
文摘Due to larger atom utilization,unique electronic properties and unsaturated coordination,atomically dispersed non-precious metal catalysts with outstanding performances have received great attention in electrocatalysis.Considering the challenge of serious aggregation,rational synthesis of an atomic catalyst with good dispersion of atoms is paramount to the development of these catalysts.Herein,we report an enhanced confinement strategy to synthesize a catalyst comprised of atomically dispersed Fe supported on porous nitrogen-doped graphitic carbon from the novel and more cross-linkable Melamine-Glyoxal Resin.Densified isolated grid trapping,excessive melamine restricting,and nitrogen anchoring are strongly combined to ensure the final atomic-level dispersion of metal atoms.Experimental studies revealed enhanced kinetics of the obtained catalyst towards oxygen reduction reaction(ORR).This catalytic activity originates from the highly active surface with atomically dispersed iron sites as well as the multi-level three-dimensional structure with fast mass and electron transfer.The enhanced confinement strategy endows the resin-derived atomic catalyst with a great prospect to develop for commercialization in future.
