Single-Mg-Atom Catalyst with a Dual Active Center as an Emerging Promising Sensing Platform.

Abstract

Bisphenol compounds [bisphenol A (BPA), etc.] are one class of the most important and widespread pollutants in food and environment, which pose severe endocrine disrupting effect, reproductive toxicity, immunotoxicity, and metabolic toxicity on humans and animals. Simultaneous rapid determination of BPA and its analogues (bisphenol S, bisphenol AF, etc.) with extraordinary potential resolution and sensitivity is of great significance but still extremely challenging. Herein, a series of single-atom catalysts (SACs) were synthesized by anchoring different metal atoms (Mg, Co, Ni, and Cu) on N-doped carbon materials and used as sensing materials for simultaneous detection of bisphenols with similar chemical structures. The Mg-based SAC enables the potential discrimination and simultaneous rapid detection of multiple bisphenols, showing outstanding analytical performances, outperforming all other SACs and traditional electrode materials. Our experiments and density functional theory calculations show that pyrrolic N serves as the adsorption site for the adsorption of bisphenols and the Mg atom serves as the active site for the electrocatalytic oxidation of bisphenols, which play a synergistic role as dual active centers in improving the sensing performance. The results of this work may pave the way for the rational design of SACs as advanced sensing and catalytic materials.