CoSex nanocrystalline-dotted CoCo layered double hydroxide nanosheets: a synergetic engineering process for enhanced electrocatalytic water oxidation.

Manipulating the electrical conductivity and morphology of Co-based (hydr)oxides is significant for optimizing energy conversion in the oxygen evolution reaction (OER). Herein, 2D CoSex nanocrystalline-dotted porous CoCo layered double hydroxide nanosheets (Co-Se NSs) were designed and synthesized via a modified in situ reduction and interface-directed assembly in an inert atmosphere. During the synchronous reduction/precipitation reaction between Co2+-oleylamine and NaHSe at the toluene-water interface, the hydrated Co-O and Co-Se clusters are generated and sequentially assemble under strong extrusion driven by the interfacial tension. Owing to the enriched vacancies on the lateral surfaces, the obtained loose and porous Co-Se NS presents low crystallinity. Moreover, electrons could spontaneously transfer from the CoCo LDH to the neighboring CoSex nanocrystallites due to the stronger electron-withdrawing capability of metallic CoSex, and thus more Co atoms in the CoCo layered double hydroxide (LDH) present a high oxidation state. This synergistic manipulation in the structure, component, and electron configuration of the Co-Se NS can increase the density of the OER active-sites, improve the electrical conductivity, and also offer a large accessible surface area and permeable channels for ion adsorption and transport. As a result, the resulting Co-Se NSs feature high catalytic activity towards OER, in particular a low onset potential of 1.48 V and an overpotential of only 290 mV at a current density of 10 mA cm-2 for the Co-Se-2 NS, as well as good stability in an accelerated durability test. The strategy developed here provides a reliable and valid way to synthesize multicomponent NSs, and is able to be extended to other areas of application.