Exploring the Pyrolysis Mechanism towards OER Performance Optimization of Salophen‐ligated Binuclear Cobalt Complex†.

Main observation and conclusion: Exploring pyrolysis process is an efficient way to study the relationship between molecular level of the precursor structure and electrocatalytic functional materials in practice. Here, the unique semi‐enclosed sector structure of Salophen ligands with highly symmetric N, N, O, O mode was introduced to construct binuclear Co complex [Co2(salophen)(Cl)2(C2H3N)] (compound 1), which provides preliminary theoretical basis for the efficient coreshell structure electrocatalysts obtained by pyrolysis regulation. Moreover, we adopted TG‐MS to real‐time track the pyrolysis process from precursors of binuclear Co complexes with Salophen ligand to efficient catalytic materials with core‐shell nanostructures. As expected, the 1‐600 sample achieves ultra‐low overpotential of 256 mV at 10 mA·cm–2 and high catalytic stability within 10 h in 1 mol/L KOH solution. This work highlights salophen‐ligated complex as excellent precursor material system for the analysis of pyrolysis evolution process, and provides an opportunity for targeted preparation of efficient oxygen evolution reaction (OER) nanocatalysts. [ABSTRACT FROM AUTHOR]