MXenes anchored Co2N/Co3O4 heterostructure with electron pulling effect promoting conversion of LiOx moieties

[Display omitted] •Theoretical prediction guided experimental modulation strategy for heterostructure.•The e- rich Co2N in heterostructure facilitated LiOx electrocatalytic conversion.•Co2N/Co3O4-Ti3C2Tx was constructed via a facile in-situ oxidation and nitriding.•Co2N/Co3O4-Ti3C2Tx improved the discharge–charge kinetics and cyclability.•Co2N/Co3O4-Ti3C2Tx had few side reactions, associated with the lower CO2 emission. The conversion of LiOx moieties was determined the kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in Li-O2 battery (LOB). Electrocatalysts with rationally modulated structures could tune the LiOx conversion and conquer the sluggish kinetics in ORR and OER. Herein, we constructed the Co2N/Co3O4-Ti3C2Tx (NCT) composite with Co2N/Co3O4 heterostructure anchored on Ti3C2Tx MXene nanosheets. The NCT was endowed with more active sites, and good conductivity, benefiting to facilitate reaction kinetics. Most importantly, the synergistic interaction via the electron pulling effect between Co2N and Co3O4 demonstrated the optimized adsorption energy towards intermediates and lower energy barrier for promoted kinetics on active Co2N. Additionally, NCT heterostructure displayed few side reactions related to Li2CO3/CO2. Consequently, it presented superior electrocatalytic activity with a low overpotential of 0.65 V and long-term durability >300 cycles. This result provided a new strategy for designing high-performance electrocatalysts and novel insight for LiOx moieties conversion.