Abstract

An electrocatalyst with heterogeneous nanostructure, especially the hierarchical one, generally shows a more competitive activity than that of its single-component counterparts for oxygen evolution reaction (OER), due to the synergistically enhanced kinetics on enriched active sites and reconfigured electronic band structure. Here this work introduces hierarchical heterostructures into a NiMo@NiS/MoS2@Ni3S2/MoOx (NiMoS) composite by one-pot controlled moderative sulfidation. The optimal solvent composition and addition of NaOH enable NiMoS to own loose and porous structures, smaller nanoparticle sizes, optimal phase composition and chemical states of elements, improving the OER activity of NiMoS. To achieve current densities of 50 and 100 mA cm−2, small overpotentials of 275 and 306 mV are required respectively, together with a minor Tafel slope of 58 mV dec−1, which outperforms most reported sulfide catalysts and IrO2. The synergistic effects in the hierarchical heterostructures expose more active sites, adjust the electronic band structure, and enable the fast charge transfer kinetics, which construct an optimized local coordination environment for high OER electrocatalytic activity. Furthermore, the hierarchical heterostructures suppress the distinct lowering of electrical conductivity and collapse of pristine structures resulted from the metal oxidation and synchronous S leaching during OER, yielding competitive catalytic stability.

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