Highly accessible Fe-N-C single-atom nanozymes with enhanced oxidase-like activity for smartphone-assisted colorimetric detection of uric acid.

Fe-N-C single-atom nanozymes (SANzymes), which exhibit the properties of well-defined atomic structures and carefully controlled coordination environments, have become a hot research topic in biomedical fields. Unfortunately, the lower accessibility and intrinsic activity of the FeN sites severely limit their enzyme-like activity. Here, a densely exposed surface FeN structure was constructed on layered nitrogen-doped hierarchical porous carbon support through two steps of pyrolysis strategy. Using a honeycomb porous carbon support, the Fe-N-C catalyst boasted a high specific surface area with numerous Fe anchoring sites and was equipped with efficiently accessible active FeN structures. The Fe edge effect could modulate the electronic structure of individual Fe atoms, thereby boosting the intrinsic oxidase-like activity of the FeN molecules. As a result, Fe-N-C SANzymes were efficiently able to catalyze O with 3,3',5,5'-tetramethylbenzidine (TMB) as a substrate, achieving higher catalytic kinetic values than previously reported SANzymes. The colorimetric sensor using Fe-N-C SANzymes further detected uric acid (UA) with a wide detection range and a low detection limit. Then the visual sensing of the colorimetric system allowed the smartphone to identify colors by HSV patterns and obtain quantitative analysis. Moreover, the developed Fe-N-C colorimetric method showed satisfactory results in clinical samples, and proved to be a simple-operated and reliable method for detection of UA. This work not only highlights the advantages of the rationally designed edge effect of iron single atoms, but also presents the promising applicability of single-atom nanozymes in clinical diagnosis and related fields.