Fe-N-C SINGLE-ATOMIC SITE CATALYSTS: ENZYME-LIKE ACTIVITIES AND BIOSENSING APPLICATIONS

Zhaoyuan Lyu

doi:10.7273/000004445

From diagnosis of life-threatening diseases to detection of biological agents in the human body and environment, biosensors are becoming a critical part of modern life. The fast detection process and accurate detection results have posed high requirements in the sensitivity and specificity of the biosensors. Recently, some nanomaterials have been found to possess unexpected peroxidase-like activities, and great progress has been made to fabricate colorimetric biosensors based on the peroxidase-like activities of these nanomaterials. These nanomaterials exhibit flexibility in structural design and composition, easy separation and storage, high stability, simple preparation, and tunable catalytic activity. Fe-based single-atomic site catalysts (SASCs), with the natural metalloproteases-like active site structure, have attracted widespread attention in biosensing applications. Precisely controlling the isolated single-atomic Fe-N-C active site density and structure is crucial to improving the SASCs’ performance. In this dissertation, different strategies are used to increase the enzyme-like activity of Fe-N-C SASCs. Using ion-imprinting technology to precisely control ions at the atomic level, form numerous well-defined single-atomic Fe-N-C sites, and achieve in situ detection of H2O2 generated from cells. The use of nanoconfinement force can greatly increase the number of Fe-Nx active sites in the material, thereby greatly improving the enzyme-like properties of the material, which can then be used for biosensing and sensitive and selective detection of disease biomarkers. Furthermore, harnessing the advantages of two-dimensional (2D) materials to synthesize SASCs can further enhance their activity, as the 2D structure can help expose more single-atomic sites that can directly participate in the reaction. This strategy has been successfully used to fabricate biosensing systems for herbicide detection. More importantly, different SASCs can be further designed by using appropriate precursors to achieve structural mimicry of the natural enzyme, through control size and morphology to achieve point-of-care detection via lateral-flow immunoassay. Fe-N-C SASCs synthesized in this work have significant potential to replace natural enzymes for high-sensitive biosensing applications. Their unique single-atomic geometrical structure exhibits significant advantages in biocatalytic activity, stability, and selectivity. We believe the continuously developed strategies can enable the Fe-N-C SASCs to explore their wider applications in various biosensing applications with excellent detection performance.

Fe-N-C SINGLE-ATOMIC SITE CATALYSTS: ENZYME-LIKE ACTIVITIES AND BIOSENSING APPLICATIONS

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