An Fe-N/S-C hybrid electrocatalyst derived from bimetal-organic framework for efficiently electrocat

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Heteroatoms doped Fe-N-C electrocatalysts have been widely acknowledged as one of the most promis-ing candidates to replace Pt-based materials for electrocatalyzing oxygen reduction reaction(ORR).However,the complicated synthesis method and controversial catalytic mechanism represent a substan-tial impediment as of today.Herein,a very facile strategy to prepare Fe-N/S-C hybrid through pyrolyzing Zn and Fe bimetallic MOFs is rationally designed.The electrocatalytic ORR performance shows a volcano-type curve with the increment of added Fe content.The half-wave potential(E1/2)for ORR at optimized Fe-N/S-C-10%(10%=n(Fe)/(n(Fe)+n(Zn)),n(Fe)and n(Zn)represent the moles of Fe2+and Zn2+in the precursors,respectively)shifts significantly to the positive direction of 19.6 mV with respect to that of Pt/C in acidic media,as well as a high 4e selectivity and methanol tolerance.After 10,000 potential cycles,E1/2 exhibits a small negative shift of~27.5 mV at Fe-N/S-C-10%compared favorably with Pt/C(~141.0 mV).This can be attributed to:(i)large specific surface area(849 m2/g)and hierarchically porous structure are favorable for the rapid mass transfer and active sites exposure;(ii)the embedded Fe-containing nanoparticles in porous carbon are difficult to be moved and further agglomerated during the electrochemical accelerated aging test,further improving its stability;(iii)there exist small Fe-containing nanoparticles,uniformly doped N and S,abundant Fe-N as efficiently active sites.This work represents a breakthrough in the development of high-efficient non-precious-metal catalysts(NPMCs)to address the current Pt-based electrocatalysts challenges.
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