Sulfur Vacancy-Rich Amorphous Rh Metallene Sulfide for Electrocatalytic Selective Synthesis of Aniline Coupled with Efficient Sulfion Degradation.

ABSTRACT

The construction of efficient and stable electrocatalysts is of widespread research significance for electrocatalytic coupling reactions. Herein, an amorphous Rh metallene sulfide with sulfur-rich vacancies (a-RhS2-x metallene) is synthesized for the cathodic nitrobenzene (Ph-NO2) electroreduction reaction (ERR) to aniline (Ph-NH2) coupled with the anodic sulfur ion (S2-) oxidation reaction (SOR) in a coelectrolysis system. On the one hand, the amorphous Rh metallene structure can provide enough of a reactive site. On the other hand, the amorphization and the introduced S vacancies can generate rich defects and ligand unsaturated sites to improve the intrinsic activity of the active sites. Due to these advantages, the a-RhS2-x metallene exhibits superior electrocatalytic performance for Ph-NO2 ERR and SOR. Inspiringly, in the assembled electrocatalytic coupling system, the required overpotential is only 0.442 V at 10 mA cm-2 to drive the cathodic Ph-NO2 ERR and anodic SOR, which allows for promising energy-efficient electrolysis to generate high value-added chemicals.