Iron Single-Atom Catalyst-Enabled Peroxydisulfate Activation Enhances Cathodic Electrochemiluminescence of Tris(bipyridine)ruthenium(II)

作者：Luo, Zhen; Xu, Weiqing; Wu, Zhichao; Jiao, Lei; Luo, Xin; Xi, Mengzhen; Su, Rina; Hu, Liuyong^*; Gu, Wenling^*; Zhu, Chengzhou^*

来源：Analytical Chemistry, 2023, 95(28): 10762-10768.

DOI：10.1021/acs.analchem.3c01822

• ELECTROGENERATED CHEMILUMINESCENCE
• DEGRADATION
• GENERATION

The tris(bipyridine)ruthenium(II) (Ru(bpy)(3) (2+))-tripropylamine anodic electrochemiluminescence(ECL) systemhas been widely applied in commercial bioanalysis. However, the presenceof amine compounds in the biological environment results in unavoidableanodic interference signals, which hinder further extensive use ofthe system. In contrast, the cathodic Ru(bpy)(3) (2+) ECL system can overcome these limitations. The Ru(bpy)(3) (2+)/peroxydisulfate (S2O8 (2-), PDS) ECL system has been extensively employed due to its abilityto produce a sulfate radical anion (SO4 (& BULL;-)) with strong oxidation ability, which enhances the ECL signal. However,the symmetrical molecular structure of PDS makes it challenging tobe activated and causes low luminescence efficiency. To address thisissue, we propose an efficient Ru(bpy)(3) (2+)-basedternary ECL system that uses the iron-nitrogen-carbonsingle-atom catalyst (Fe-N-C SAC) as an advanced accelerator.Fe-N-C SAC can efficiently activate PDS into reactiveoxygen species at a lower voltage, which significantly boosts thecathodic ECL emission of Ru(bpy)(3) (2+). Benefitingfrom the outstanding catalytic activity of Fe-N-C SAC,we successfully established an ECL biosensor that detects alkalinephosphatase activity with high sensitivity, demonstrating the feasibilityof practical application.

• 单位
  武汉工程大学