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

• Published in: ACS nano 2023-01, Vol.17 (1), p.790-800
• Main Authors: Mao, Qiqi, Mu, Xu, Deng, Kai, Yu, Hongjie, Wang, Ziqiang, Xu, You, Li, Xiaonian, Wang, Liang, Wang, Hongjing
• Format: Article
• Language: English
• ISSN: 1936-0851; 1936-086X
• DOI: 10.1021/acsnano.2c11094

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.