Luminol-based electrochemiluminescence (ECL) can be readily excited by various reactive oxygen species (ROS) electrogenerated with an oxygen reduction reaction (ORR). However, the multiple active intermediates involved in the ORR catalyzed with complex nanomaterials lead to recognizing the role of ROS still elusive. Moreover, suffering from the absence of the direct electrochemical oxidation of luminol at the cathode and poor transformation efficiency of O2 to ROS, the weak cathodic ECL emission of luminol is often neglected. Herein, owing to the tunable coordination environment and structure-dependent catalytic feature, single-atom catalysts (SACs) are employed to uncover the relationship between the intrinsic ORR activity and ECL behavior. Interestingly, the traditionally negligible cathodic ECL of luminol is first boosted (ca. 70-fold) owing to the combination of electrochemical ORR catalyzed via SACs and chemical oxidation of luminol. The boosted cathodic ECL emission exhibits electron-transfer pathway-dependent response by adjusting the surrounding environment of the center metal atoms in a controlled way to selectively produce different active intermediates. This work bridges the relationship between ORR performance and ECL behavior, which will guide the development of an amplified sensing platform through rational tailoring of the ORR activity of SACs and potential-resolved ECL assays based on the high-efficiency cathodic ECL reported.
Noble metal based nanozymes show great potential in replacing natural enzymes; however, their development is greatly restricted by their relatively low specificity and activity. Herein, we report the synthesis of a class of amorphous/crystalline PtRuTe nanomaterials with a Pt/Te-enriched core and a Ru-enriched shell as efficient peroxidase mimics with selectively enhanced peroxidase-like activity and suppressed oxidase-like activity. We demonstrate that amorphous domains play a critical role in tuning and optimizing the catalytic properties. The PtRuTe nanozyme with high-percentage defects exhibits superior catalytic activities and kinetics, and the suppressed oxidase-like activity could diminish the interference of O 2 in the glucose colorimetric assay. The high catalytic performance can be caused by amorphous phase induced electron redistribution and electronic interactions between different elements and the synergistic effect of multimetallic nanocrystals. The concurrent extraordinary peroxidase-like activity and suppressed oxidase-like activity guarantee the amorphous/crystalline PtRuTe nanozymes as promising alternatives of natural enzymes for biosensing and beyond.
All-inorganic halide perovskite nanocrystals with their fascinating optical properties have drawn increasing attention as promising nanoemitters. However, due to the intrinsic poor colloidal stability against the external environment, the practical applications are greatly limited. Herein, a facile and effective strategy for the in situ encapsulation of CsPbBr3 NCs into highly dense multichannel polyacrylonitrile (PAN) nanofibers via a uniaxial electrospinning strategy is presented. Such a facile uniaxial electrospinning strategy enables the in situ formation of CsPbBr3 NCs in PAN nanofibers without the introduction of stabilizers. Significantly, the obtained CsPbBr3 nanofibers not only display intense fluorescence with a high quantum yield (≈48%) but also present high stability when exposed to water and air owing to the peripheral protecting matrix of PAN. After immersing CsPbBr3@PAN nanofiber films in water for 100 days, the quantum yield of CsPbBr3@PAN nanofibers maintained 87.5% of the original value, which was much higher than that using CsPbBr3 NCs. Furthermore, based on the spectral overlap between the electrochromic material of ruthenium purple and fluorescence of CsPbBr3@PAN nanofiber films with excellent water stability, a reversible fluorescence switch is constructed with good fatigue resistance, suggesting their promising applications.
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