Trifunctional Graphene‐Sandwiched Heterojunction‐Embedded Layered Lattice Electrocatalyst for High Performance in Zn‐Air Battery‐Driven Water Splitting

Zn-air battery (ZAB)-driven water splitting holds great promise as a next-generation energy conversion technology, but its large overpotential, low activity, and poor stability for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER) remain obstacles. Here, a trifunctional graphene-sandwiched, heterojunction-embedded layered lattice (G-SHELL) electrocatalyst offering a solution to these challenges are reported. Its hollow core-layered shell morphology promotes ion transport to Co₃S₄ for OER and graphene-sandwiched MoS₂ for ORR/HER, while its heterojunction-induced internal electric fields facilitate electron migration. The structural characteristics of G-SHELL are thoroughly investigated using X-ray absorption spectroscopy. Additionally, atomic-resolution transmission electron microscopy (TEM) images align well with the DFT-relaxed structures and simulated TEM images, further confirming its structure. It exhibits an approximately threefold smaller ORR charge transfer resistance than Pt/C, a lower OER overpotential and Tafel slope than RuO₂, and excellent HER overpotential and Tafel slope, while outlasting noble metals in terms of durability. Ex situ X-ray photoelectron spectroscopy analysis under varying potentials by examining the peak shifts and ratios (Co²⁺/Co³⁺ and Mo⁴⁺/Mo⁶⁺) elucidates electrocatalytic reaction mechanisms. Furthermore, the ZAB with G-SHELL outperforms Pt/C+RuO₂ in terms of energy density (797 Wh kg^-1) and peak power density (275.8 mW cm^-2), realizing the ZAB-driven water splitting.