Sulfidation and NaOH etching in CoFeAl LDH evolved catalysts for an efficient overall water splitting in an alkaline solution

In this study, a hierarchical interconnected porous metal sulfide heterostructure was synthesized from CoFeAl layered double hydroxides (LDHs) by a two-step hydrothermal process (sulfidation and a NaOH etching process). Among the as-made samples, the CoFeAl-T-NaOH electrode exhibited excellent oxygen and hydrogen evolution reaction catalytic activities with overpotentials of 344 mV and 197 mV at the current density of 100 mA cm^-2, respectively. Meanwhile, small Tafel slopes of 57.7 mV dec^-1 and 106.5 mV dec^-1 for water oxidation and hydrogen evolution were observed for the CoFeAl-T-NaOH, respectively. Serving as both the cathode and anode for overall water splitting, the CoFeAl-T-NaOH electrode reached a current density of 10 mA cm^-2 at a cell voltage of 1.65 V with excellent stability. The enhanced electrocatalytic activity could be attributed to: the hierarchical interconnected nanosheet structure facilitating mass transport; the porous structure promoting electrolyte infiltration and reactant transfer; the heterojunction accelerating charge transfer; and the synergistic effect between them. This study offered a new clue for in situ synthesizing porous transition-metal based heterojunction electrocatalysts with a careful tuning of the sequence of sulfuration and alkaline etching to enhance the electrocatalytic performance.