Cerium oxide boosted CoFe-N codoped carbon nanotubes with abundant oxygen-vacancies toward efficient oxygen reduction and methanol oxidation reaction

In this study, we designed a novel strategy that utilizes N-doped carbon nanotubes as the chemical bond supporter to stabilize ultrafine CoFe alloy and introduces secondary CeO2 active sites into the hybrid, resulting in the formation of CeO2/CoFe-NCNTs heterostructures with exceptional bifunctional electrocatalytic capabilities. To be specific, solution dispersion and high-temperature calcination methods were employed to create the CoFe-NCNTs active sites through the introduction of ethylenediamine into the network interstitials of Co-EDTA and Fe-EDTA. The CeO2/CoFe-NCNTs hybrid not only promotes oxygen absorption and conversion of intermediates, but also accelerates charge transfer capability, thus enhancing oxygen reduction reaction (ORR) performance, while simultaneously inducing boosted the methanol oxidation reaction (MOR) activity. Moreover, the well-dispersed CoFe nanoparticles within the hybrid hold significant potential for establishing metal-nitrogen bonds with the N-doped carbon nanotube network, resulting in efficient catalytic behavior driven by synergistic effects with CeO2 nanoparticles, which contributes to reactant activation. As expected, the resultant CeO2/CoFe-NCNTs-2 exhibits remarkable electrocatalytic performance, with a current density of 281.40 mA cm−2 at a scan rate of 200 mV s−1 and a low Tafel slope (71.3 mV dec−1) for MOR, as well as achieving excellent half-wave potential and onset potential values of 0.834 and 0.90 V (vs. RHE) for ORR. Additionally, it exhibits durable cycle stability for both MOR and ORR, retaining 92.8% and 96.4% of its initial current density during the I-t test, respectively. This work establishes a highly efficient bifunctional earth-abundant electrocatalysts for both anode and cathode reactions in methanol fuel cells.