Abstract
Efficient oxygen evolution reaction catalysts can be prepared via controlled pyrolysis of molecular platforms, and there is still minimal mechanistic understanding of such pyrolysis processes. Here, we introduce a 3-MeOsalophen-ligated cobalt complex as a precursor to obtain a Co-based OER electrocatalyst via controlled pyrolysis under an inert atmosphere. In our case, the unique N, O chelation mode of the 3-MeOsalophen ligand (bis[3-methoxysalicylydene]-1,2 iminophenylenediamine) was used to synthesis a Co(2) complex [Co(2)(3-MeOsalophen)(Cl)(3)(CH(3)OH)(2)]. By regulating the pyrolysis conditions, we successfully obtained a N-doped carbon Co/CoO (x) core-shell nanostructure. More importantly, TG-MS was first adopted for tracking the decomposition products of the complex in the pyrolysis process, further finding out the evolution mechanism from Co(2) to the core-shell nanostructure. As an electrocatalyst for the oxygen evolution reaction, the core-shell Co/CoO (x) @NC-800 nanostructure achieves an ultralow overpotential of 288 mV at 10 mA cm(-2) in 1 M KOH solution. This work offers guiding insight into controlled pyrolysis via TG-MS analysis, using a novel complex precursor for precise regulation of heteroatom-doped (3d) transition metal-based electrocatalysts.