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To develop high-performance and low-cost electrocatalysts for the oxygen reduction reaction (ORR) in Al-air batteries, a promising hierarchical porous N,S-codoped carbon architecture with cobalt-nickel-sulphide nanoparticles immobilized inside was prepared using a simple double-phase encapsulation approach (DPEA), followed by a post heat treatment. The integrated hybrid architecture (Ni-Co-S@G/NSC) exhibited not only a comparable onset potential (0.94 V vs. RHE) and half-wave potential (0.86 V vs. RHE) but also a higher discharge voltage plateau (∼1.23 V at discharge current density of 150 mA cm −2 ) with superior stability to the commercial Pt/C catalyst in ORR and the full cell test. A combination of structural characterizations (e.g., XPS, RSS, XRD, SEM, HRTEM, and BET) and electrochemical analyses showed that the high ORR activity of the Ni-Co-S@G/NSC catalyst was attributed to its high surface area and pore volume, proper degree of the graphitization, and high content of active species combined with their synergetic interactions. Our findings show the advantages in utilizing a metal-organic framework with DPEA for designing well-dispersed, highly active and robust N,S-codoped porous carbons immobilized with sulphide NP catalysts for Al-air batteries. [ABSTRACT FROM AUTHOR]

[Display omitted] • NiMn 2 O 4 -based Ni-Mn bimetallic oxides were fabricated. • The Ni-Mn bimetallic oxides access excellent ORR catalytic performance. • The Ni-Mn bimetallic oxides exhibit good discharge performance in Al-air battery. • Ni-Mn-600 has nanorod morphology and high ratio of (Mn3++Mn4+)/Mn2+ and Ni3+/Ni2+. To date, research on air battery catalysts has been mainly focused on finding materials with a high oxygen reduction reaction (ORR) catalytic activity. However, the high cost of platinum catalysts restricts their commercialization. Herein, we report a simple hydrothermal-calcination method to fabricate low-cost NiMn 2 O 4 -based Ni-Mn bimetallic oxides. The Ni-Mn-600 sample showed a high onset potential (1.01 V vs. RHE), which was more positive than that for 20 wt% Pt/C (0.97 V vs. RHE), and its half-wave potential (0.78 V vs. RHE) was comparable to that for 20 wt% Pt/C (0.84 V vs. RHE). Moreover, Ni-Mn-600 as an Al-air battery air–cathode catalyst exhibited a high discharge plateau of 1.42 V and peak power density of 100.45 mW cm−2, which outperformed those for 20 wt% Pt/C (1.34 V and 76.10 mW cm−2). The high ORR electrocatalytic activity of Ni-Mn-600 may be attributed to the nanorod morphology and high ratio of (Mn3++Mn4+)/Mn2+ and Ni3+/Ni2+. This work demonstrated that NiMn 2 O 4 -based Ni-Mn bimetallic oxides as cathode catalysts have good research prospects in aluminum-air batteries and other energy applications. [ABSTRACT FROM AUTHOR]