Carbon quantum dots (CQDs) with their strong photoluminescence (PL) activity, high biocompatibility, robust stability, low cytotoxicity, and flexible surface structures have been employed in many fields including chemical sensing, biosensing, photocatalyst, energy storage, and biomedical applications. Of note, CQDs present an intrinsic pH-sensitive PL nature indicating their intense potential for pH-mediated sensing and imaging. Despite the numerous studies performed in the last two decades, the pH-sensitive PL mechanism of CQDs is still under debate and must be clarified to overcome the limitations in practical applications. Therefore, in this report, we performed a systematical study to determine the pH-sensitive PL nature of boron/nitrogen co-doped CQDs (B/N CQDs). In the first part, B/N CQDs with a strong blue emission were fabricated via a hydrothermal synthesis procedure. B/N-CQDs showed a strong blue PL emission with high quantum yield and excitation-dependent nature. Under the low pH conditions (pH 3), B/N-CQDs exhibited a robust green fluorescence emission with a significant red-shift (48 nm) and the loss of the excitation-dependent nature. The change in PL nature originated from the protonation of surface groups, a decrease in negative surface charge (from −20.6 to −1.23 eV), and finally, aggregation of the nanostructure (the size of CQDs from 4.8 to 7.5 nm). However, in the case of alkaline conditions, the deprotonation surface groups significantly enhanced the surface charge and led to the emergence of a negative ‘protective shell’ with a zeta potential of −71.3 eV. In a high pH medium (pH 13), PL spectra showed the loss of excitation-dependent features and a red-shift (35 nm) in emission peak maxima with lower intensity. This report provides significant progress in the clarification of the pH-sensitive PL mechanism of CQDs. We envision that the proposed CQDs would provide unique opportunities in the fabrication of novel pH sensor systems and fluorescence imaging where a wide range of pH sensitivity is required.
In the last two decades, fluorescent carbon quantum dots (CQDs) have attracted intense interest as a new fluorescent nanomaterial with unique properties. This material offers significant advantages compared with conventional dyes and inorganic QD systems, and is used extensively in many different fields, especially in bioimaging and sensor applications. Despite all the positive values they offer, the production of CQD systems with excitation wavelength-dependent nature and high quantum yield (QY) is still a scientific challenge. In this study, we proposed the fabrication of CQD through a facile and easy-to-tune hydrothermal method using cheap and biocompatible precursors such as urea and lactic acid. The effect of experimental parameters including synthesis time, temperature, and mass ratio of the precursors, were determined to obtain the highest QY (48%). The as-prepared nitrogen-doped (N-doped) CQDs exhibited robust stability in the dark and in a wide range of pH values with excitation wavelength-dependent properties. Additionally, CQDs showed remarkable sensitivity and selectivity in the sensing of Fe3+ in blood plasma with a linear correlation in the range of 0–1000 μM, indicating the high potential of CQDs in practical applications. Lastly, cytotoxicity and antibacterial activity tests demonstrated the low toxicity and high biocompatibility of proposed CQDs. Considering the facile and efficient synthetic method, easy-to-tune optical properties, excitation-dependent nature, high fluorescence activity, and low cytotoxicity, we strongly anticipate that N-doped CQDs could provide unique advantages in various biomedical applications including diagnosis, bioimaging, and biosensors.
Oxygen vacancies in tungsten trioxide (WO3) nanostructures (WO3−x) dominate the major characteristics of the material and determine their activity in various applications including photocatalysis and surface-enhanced Raman spectroscopy (SERS).
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