2026/02/18 by Yin Zhou, Kun Yin, Tian Zhang +14 · 1 voice
Engineering · #Advanced Battery Materials and Technologies #Advancements in Battery Materials #Advanced battery technologies research
paper · pdf · doi:10.1007/s40820-026-02085-z
openalex publication_date 2026/02/18 · openalex created_date 2026/02/19 · openalex updated_date 2026/07/29
Abstract Elucidating the structure–activity relationship between the electronic structure of catalytic active sites and oxygen evolution reaction (OER) activity at the orbital level is critical yet challenging in lithium–oxygen (Li–O 2 ) batteries. Herein, employing frontier molecular orbital theory, we designed a Pt-based catalyst as a model cathode to investigate the influence of frontier orbital interactions between the Pt d z 2 orbital and the 5 σ orbital of LiO 2 on the OER activity. Specifically, compared to the pure Pt catalyst, the d z 2 – d z 2 orbital coupling between low-electronegativity Fe and Pt in PtFe catalyst induces predominant electron transfer from Fe to the d z 2 frontier orbital of Pt. As the Pt content in PtFe alloys increases progressively (from Pt 58 Fe 42 , Pt 67 Fe 33 to Pt 76 Fe 24 ), the electron population of the Pt 5 d z 2 orbital gradually decreases (1.92 for Pt 58 Fe 42 , 1.85 for Pt 67 Fe 33 , and 1.80 for Pt 76 Fe 24 ). This leads to a gradual enhancement in the strength of interactions between the Pt d z 2 orbital and the frontier orbitals of LiO 2 , consequently resulting in a progressive decline in the OER catalytic activity. Establishing the correlating between the electron population in the d z 2 frontier orbital and OER activity provides a descriptor for designing efficient electrocatalysts in Li–O 2 batteries.