Single-atom catalysts have attracted
numerous attention due to
the high utilization of metallic atoms, abundant active sites, and
highly catalytic activities. Herein, a single-atom ruthenium biomimetic
enzyme (Ru-Ala-C3N4) is prepared by dispersing
Ru atoms on a carbon nitride support for the simultaneous electrochemical
detection of dopamine (DA) and uric acid (UA), which are coexisting
important biological molecules involving in many physiological and
pathological aspects. The morphology and elemental states of the single-atom
Ru catalyst are studied by transmission electron microscopy, energy
dispersive X-ray elemental mapping, high-angle annular dark field–scanning
transmission electron microscopy, and high-resolution X-ray photoelectron
spectroscopy. Results show that Ru atoms atomically disperse throughout
the C3N4 support by Ru–N chemical bonds.
The electrochemical characterizations indicate that the Ru-Ala-C3N4 biosensor can simultaneously detect the oxidation
of DA and UA with a separation of peak potential of 180 mV with high
sensitivity and excellent selectivity. The calibration curves for
DA and UA range from 0.06 to 490 and 0.5 to 2135 μM with detection
limits of 20 and 170 nM, respectively. Moreover, the biosensor was
applied to detect DA and UA in real biological serum samples using
the standard addition method with satisfactory results.
Uric acid (UA) detection is essential in diagnosis of arthritis, preeclampsia, renal disorder, and cardiovascular diseases, but it is very challenging to realize the required wide detection range and low detection limit. We present here a single-atom catalyst consisting of Co(II) atoms coordinated by an average of 3.4 N atoms on an N-doped graphene matrix (A–Co–NG) to build an electrochemical biomimetic sensor for UA detection. The A–Co–NG sensor achieves a wide detection range over 0.4–41,950 μM and an extremely low detection limit of 33.3 ± 0.024 nM, which are much better than previously reported sensors based on various nanostructured materials. Besides, the A–Co–NG sensor also demonstrates its accurate serum diagnosis for UA for its practical application. Combination of experimental and theoretical calculation discovers that the catalytic process of the A–Co–NG toward UA starts from the oxidation of Co species to form a Co3+–OH–UA*, followed by the generation of Co3+–OH + *UA_H, eventually leading to N–H bond dissociation for the formation of oxidized UA molecule and reduction of oxidized Co3+ to Co2+ for the regenerated A–Co–NG. This work provides a promising material to realize UA detection with wide detection range and low detection limit to meet the practical diagnosis requirements, and the proposed sensing mechanism sheds light on fundamental insights for guiding exploration of other biosensing processes.
Instability of 2D phosphorene material is the major obstacle for its broad applications. Herein phosphorene is sandwiched with self-assembled iron porphyrin monolayers on both sides (I-Phene) to significantly enhance stability. Iron porphyrin has strong interaction with phosphorene through formation of P-Fe bonds. The sandwich structure offers excellent stability of phosphorene by both-sided monolayer protections for an intact phosphorene structure more than 40 days under ambient conditions. Meanwhile, the electron transfer between iron porphyrin and phosphorene result in a high oxidation state of Fe, making I-Phene biomimetic sensitivity toward oxidation of nitric oxide (NO) for 2.5 and 4.0 times higher than phosphorene and iron-porphyrin alone, respectively. Moreover, I-Phene exhibits excellent selectivity, a wide detection range, and a low detection limit at a low oxidation potential of 0.82 V, which is comparable with the reported noble metal based biomimetic sensors while ranking the best among all non-noble biomimetic ones. I-Phene is further used for real-time monitoring NO released from cells. This work provides effective approach against phosphorene degrading for outstanding stability, which has universal significance for its various important applications, and holds a great promise for a highly sensitive biomimetic sensor in live-cell assays.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.