Fe3C-Assisted Single Atomic Fe Sites for Sensitive Electrochemical Biosensing

化学 电化学 催化作用 生物传感器 纳米技术 活动站点 检出限 金属 碳纳米管 密度泛函理论 纳米晶 电极 计算化学 物理化学 材料科学 生物化学 色谱法 有机化学
作者
Xiaoqian Wei,Shaojia Song,Weiyu Song,Weiqing Xu,Lei Jiao,Xin Luo,Nannan Wu,Hongye Yan,Xiaosi Wang,Wenling Gu,Lirong Zheng,Chengzhou Zhu
出处
期刊:Analytical Chemistry [American Chemical Society]
卷期号:93 (12): 5334-5342 被引量:75
标识
DOI:10.1021/acs.analchem.1c00635
摘要

The rational construction of advanced sensing platforms to sensitively detect H2O2 produced by living cells is one of the challenges in both physiological and pathological fields. Owing to the extraordinary catalytic performances and similar metal coordination to natural metalloenzymes, single atomic site catalysts (SASCs) with intrinsic peroxidase (POD)-like activity have shown great promise for H2O2 detection. However, there still exists an obvious gap between them and natural enzymes because of the great challenge in rationally modulating the electronic and geometrical structures of central atoms. Note that the deliberate modulation of the metal–support interaction may give rise to the promising catalytic activity. In this work, an extremely sensitive electrochemical H2O2 biosensor based on single atomic Fe sites coupled with carbon-encapsulated Fe3C crystals (Fe3C@C/Fe–N–C) is proposed. Compared with the conventional Fe SASCs (Fe–N–C), Fe3C@C/Fe–N–C exhibits superior POD-like activity and electrochemical H2O2 sensing performance with a high sensitivity of 1225 μA/mM·cm2, fast response within 2 s, and a low detection limit of 0.26 μM. Significantly, sensitive monitoring of H2O2 released from living cells is also achieved. Moreover, the density functional theory calculations reveal that the incorporated Fe3C nanocrystals donate electrons to single atomic Fe sites, endowing them with improved activation ability of H2O2 and further enhancing the overall activity. This work provides a new design of synergistically enhanced single atomic sites for electrochemical sensing applications.
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