摘要
Modulation of metal sites coordination can significantly refine the electronic architecture of catalysts,thereby improving their catalytic performance.This work successfully developed a core–shell Co@N-doped porous carbon(Co@NC)catalyst by pyrolyzing the COF/MOF(IISERP-COF3/ZIF-67)composite in an inert atmosphere.The Co@NC catalyst exhibited impressive oxygen evolution reaction(OER)performance,with a small overpotential of 304 mV and a modest Tafel slope of 88.6 mV·dec^(−1) in a 1 M KOH,alongside remarkable stability,maintaining 98.5%of its activity over 13 h.The role of IISERP-COF3 was pivotal in preventing Co atom aggregation during the ZIF-67 pyrolysis,which facilitated the creation of mesopores for enhanced mass transport and conductivity.Moreover,it effectively modulated the Co-N coordination to fine-tune the electronic structure,thereby optimizing the catalyst's capacity for adsorption of intermediates and boosting its intrinsic activity.Density functional theory(DFT)studies corroborate that the exceptional OER efficiency of Co@NC can be linked to the enhanced Co-N coordination,optimizing the localized electronic structure at the Co active sites.This study not only proposes an innovative approach for optimizing COF/MOF as effective electrocatalysts but also clears the path for the emergence of affordable,high-performance alternatives to precious metal-based catalysts,marking a significant advancement in sustainable energy technologies.
基金
supported by the Platform of Science and Technology and Talent Team Plan of Guizhou province(No.GCC[2023]007)
the National Natural Science Foundation of China(No.52062003).
