Atomically dispersed Ru3 site catalysts for electrochemical sensing of small molecules

作者:Wu, Nannan; Zhong, Hong; Zhang, Yu; Wei, Xiaoqian; Jiao, Lei; Wu, Zhichao; Huang, Jiajia; Wang, Hengjia; Beckman, Scott P.; Gu, Wenling; Zhu, Chengzhou*
来源:Biosensors and Bioelectronics, 2022, 216: 114609.
DOI:10.1016/j.bios.2022.114609

摘要

Rational design and construction of electrochemical sensing platforms with high sensitivity and selectivity is one of the challenges in practical application. Although single-atom catalysts (SACs) have attracted extensive attention, atomically dispersed metal catalysts (ADCs) with multi-atom sites can further compensate for the deficiencies of SACs, which have gradually been a research hotspot in recent years. Herein, atomically dispersed Ru3 site catalyst (Ru-3/NC) is employed to catalyze small biomolecule oxidation, which exhibits much superior electrocatalytic ability of uric acid (UA) to Ru single-atom catalyst (Ru-1/NC). What's more, theoretical calcu-lations reveal that the enhanced performance is mainly derived from the dominant electronic structure of ADCs with multi-atom sites compared to SACs, leading to the more favorable adsorption of hydroxy anion groups, which can serve as one part of the active moiety and "promoter " to achieve the fast oxidation of small bio-molecules. Our findings provide a new paradigm for designing promising catalysts to realize highly sensitive and selective small biomolecule detection and explore the catalytic mechanisms of small biomolecules at the atomic scale.