化学
催化作用
电化学发光
级联
鲁米诺
抗坏血酸
检出限
金属
无机化学
组合化学
纳米技术
光化学
有机化学
材料科学
食品科学
色谱法
作者
Daixin Ye,Jingwei Xue,Jian Cai,Conghui Xu,Ruyan Fu,Hongbin Zhao,Jing‐Juan Xu,Wei Zhao
标识
DOI:10.1021/acs.analchem.3c00891
摘要
Single-atom catalysts (SACs), a novel kind of electrocatalysts with full metal utilization, have been developed as unique signal amplifiers in several sensing platforms. Herein, based on theoretical prediction of the oxygen reduction reaction (ORR) mechanism on different atom sites, we constructed dual-atomic-site catalysts (DACs), Fe/Mn–N–C, to catalyze luminol-dissolved oxygen electrochemiluminescence (ECL). Computational simulation indicated that the weak adsorption of OH* on a single Fe site was overcome by introducing Mn as the secondary metallic active site, resulting in a synergic dual-site cascade mechanism. The superior catalytic activity of Fe/Mn–N–C DACs for the ORR was proven by the highly efficient cathodic luminol ECL, surpassing the performance of single-site catalysts (SACs), Fe–N–C and Mn–N–C. Furthermore, the ECL system, enhanced by a cascade reaction, exhibited remarkable sensitivity to ascorbic acid, with a detection limit of 0.02 nM. This research opens up opportunities for enhancing both the ECL efficiency and sensing performance by employing a rational atomic-scale design for DACs.
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