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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]

The bond order and packing ratios in the single-crystal of the two structural polymorphs as well as the detailed electronic structures of the molecular model were studied using density functional theory. The strength of different Mn coordination bonds was analyzed in detail through Mayer bond order. Besides bond length, many other factors such as the orientation of ligand and nature of metal also significantly influence the bond order. Packing ratios calculated using cluster model reveals that packing along b direction in Dimer is more favorable than other directions due to the associated interactions of π-π and Cl...H when packing in this direction. Electronic structure helps explain the formation of Dimer from monomer or direct forming of Chain from ligand/Cl and metal. This would shed light on further understanding the importance of supramolecular interaction on crystal engineering. [ABSTRACT FROM AUTHOR]

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]