Constructing double heterojunctions on 1T/2H‑MoS2@Co3S4 electrocatalysts for regulating Li2O2 formation in lithium‑oxygen batteries
Peer-Reviewed Publication
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Co3S4 electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction (OER) activity, yet challenges remain in fabricating rechargeable lithium-oxygen batteries (LOBs) due to their poor OER performance, resulting from poor electrical conductivity and overly strong intermediate adsorption. In this work, fancy double heterojunctions on 1T/2H-MoS2@Co3S4 (1T/2H-MCS) were constructed derived from the charge donation from Co to Mo ions, thus inducing the phase transformation of MoS2 from 2H to 1T. The unique features of these double heterojunctions endow the 1T/2H-MCS with complementary catalysis during charging and discharging processes. It is worth noting that 1T-MoS2@Co3S4 could provide fast Co–S–Mo electron transport channels to promote ORR/OER kinetics, and 2H-MoS2@Co3S4 contributed to enabling moderate eg orbital occupancy when adsorbed with oxygen-containing intermediates. On the basis, the Li2O2 nucleation route was changed to solution and surface dual pathways, improving reversible deposition and decomposition kinetics. As a result, 1T/2H-MCS cathodes exhibit an improved electrocatalytic performance compared with those of Co3S4 and MoS2 cathodes. This innovative heterostructure design provides a reliable strategy to construct efficient transition metal sulfide catalysts by improving electrical conductivity and modulating adsorption toward oxygenated intermediates for LOBs.
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