“…Homogeneous Co–N–C SAs on nitrogen-doped porous carbon synthesized by a sacrificed ZIF-template method was reported to have high sensitivity and low LODs of 70 nM and 60 nM for glutathione and cysteine, respectively. 255 The Co SACs show 11-fold higher oxidase-like activity than that of Co NPs. In addition, the SACs also exhibit good selectivity among 12 kinds of other amino acids with 10 times higher concentrations.…”
This review summarizes the sensing mechanism, design strategies, structural and performance advantages of single-atom catalysts and their sensing applications.
“…Homogeneous Co–N–C SAs on nitrogen-doped porous carbon synthesized by a sacrificed ZIF-template method was reported to have high sensitivity and low LODs of 70 nM and 60 nM for glutathione and cysteine, respectively. 255 The Co SACs show 11-fold higher oxidase-like activity than that of Co NPs. In addition, the SACs also exhibit good selectivity among 12 kinds of other amino acids with 10 times higher concentrations.…”
This review summarizes the sensing mechanism, design strategies, structural and performance advantages of single-atom catalysts and their sensing applications.
“…It should be noted that there are other metal sites such as Pt, 120 Pd, 121 Zn, 122 Co, 123 Cu, 124 and so on 125 . These non‐Fe‐based SACs have yet been extensively studied.…”
Biosensors featuring single molecule detection present huge opportunities as well as challenges in food safety inspection, disease diagnosis, and environmental monitoring. Single-molecule detection is largely lacking of high enough activity, precision molecule selectivity, and understanding in the exact operating mechanism. Single-atom catalysts (SACs), especially those metals-nitrogen-carbon that mimic the natural metalloenzyme structure, and with well-defined metal atom bond configurations, high level of molecular selectivity, and easy fabrication, endow single molecule detections with practical-use feasibilities. The recent advances in singleatom catalysts also present new pathways in the key mechanism understandings. In this short review, we will first visit the brief history and advantages of SACs that have been explored only recently for moleculescale biosensors, where they are analogous and also differentiated from those nanozymes and natural metalloenzymes. Their applications in electrochemical, photochemical, and photoelectrochemical sensors are then discussed comprehensively by focusing on the different molecule-scale sensing modes in achieving local coordination-modulated signal amplifications. Finally, we identify new opportunities and challenges faced by these SACs-based single molecule detections in the further development of biosensors.
“…18a), which was believed to be important for the oxidase-like activity of single-atom nanozymes 31 . The binding environments of 18c) 36 . Thus, the local Fe electronic structure could be effectively modulated by the coordination environments, thereby potentially tailoring the electron transfer and affecting their oxidase-like activity.…”
Section: Synthesis and Characterization Of Pfesanmentioning
Inspired by structures of natural metalloenzymes, a biomimetic synthetic strategy was developed for scalable synthesis of porous Fe-N3 single atom nanozymes (pFeSAN) using hemoglobin as Fe-source and template. pFeSAN delivered 3.3- and 8791-fold higher oxidase-like activity than Fe-N4 and Fe3O4 nanozymes. The high catalytic performance is attributed to (1) the suppressed aggregation of atomically dispersed Fe; (2) facilitated mass transfer and maximized exposure of active sites for the created mesopores by thermal removal of hemoglobin (2~3 nm); and (3) unique electronic configuration of Fe-N3 for the oxygen-to-water oxidation pathway (analogy with natural cytochrome c oxidase). The pFeSAN was successfully demonstrated for the rapid colorimetric detection of glutathione with a low limit of detection (2.4 nM) and wide range (50 nM–1 mM), and further developed as a real-time, facile, rapid (~6 min) and precise visualization analysis methodology of tumors via glutathione level, showing its potentials for diagnostic and clinic applications.
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