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

Mao, Qiqi; Mu, Xu; Deng, Kai; Yu, Hongjie; Wang, Ziqiang; Xu, You; Li, Xiaonian; Wang, Liang et al. · ACS Nano · 2023

basic_science · Level V

Where this comes from

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 (<i>a</i>-RhS<sub>2-<i>x</i></sub> metallene) is synthesized for the cathodic nitrobenzene (Ph-NO<sub>2</sub>) electroreduction reaction (ERR) to aniline (Ph-NH<sub>2</sub>) coupled with the anodic sulfur ion (S<sup>2-</sup>) 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 <i>a</i>-RhS<sub>2-<i>x</i></sub> metallene exhibits superior electrocatalytic performance for Ph-NO<sub>2</sub> ERR and SOR. Inspiringly, in the assembled electrocatalytic coupling system, the required overpotential is only 0.442 V at 10 mA cm<sup>-2</sup> to drive the cathodic Ph-NO<sub>2</sub> ERR and anodic SOR, which allows for promising energy-efficient electrolysis to generate high value-added chemicals.