One-step hydrothermal synthesis of WS2 quantum dots as fluorescent sensor for sensitive and selective recognition of hemoglobin and cardiac biomarker myoglobin.

Transition metal dichalcogenide (TMD) dots exhibit excellent photoluminescence performance due to the quantum confinement effect and edge effect, and are extensively applied in electronic and optical devices, sensors, catalysis, and bioimaging. In this work, WS2 quantum dots (WS2 QDs) were prepared under a simple one-step hydrothermal method by optimizing the reaction conditions, and a quantum yield of 11.23% was achieved. The as-prepared WS2 QDs possess good photo-bleaching resistance, salt tolerance, and pH stability. The fluorescence investigations showed that the WS2 QDs acted as a highly efficient fluorescent sensor to detect hemoglobin (Hb) and cardiac biomarker myoglobin (Myo). The linear range was 1-600 µg/mL for Hb and 0.01-120 µg/mL for Myo, with detection limits as low as 260 and 7.6 ng/mL, respectively. Importantly, the WS2 QDs were used to determine the Hb/Myo content in human blood/serum samples, with satisfactory results, indicating that this technique holds promise for application in clinical diagnosis associated with Hb/Myo levels. To the best of our knowledge, this is the first example of TMD QDs without any modification as a fluorescent sensor for detecting Hb and Myo simultaneously.

Intercalating of AIEgens into MoS2 nanosheets to induce crystal phase transform for enhanced photothermal and photodynamic synergetic anti-tumor therapy.

A MoS2-based nanotherapeutic platform was developed for synergetic photothermal and photodynamic anti-tumor therapy. AIEgens TFPy-SH molecules were intercalated into MoS2 nanosheets (MoS2 NSs) with S-deficiencies to give the nanocomposite MoS2-TFPy. The AIEgens intercalation expanded the interlayer spacing of MoS2 NSs and induced the transform of MoS2 crystal phase from 2H to 1T, offering MoS2-TFPy nanocomposite high molar absorption coefficient (5.65 L g-1 cm-1), excellent photothermal conversion efficiency under near-infrared (NIR) laser irradiation (38.3%), and favorable intracellular reactive oxygen species (ROS) generation capacity. The positively charged MoS2-TFPy were mainly distributed in mitochondria after cell up-taking, and achieved 1+1>2 anti-tumor effect attributed to its favorable photothermal and photodynamic properties. The high structure and physiological stability, favorable biocompatibility, excellent photothermal and photodynamic therapy effect make the MoS2-TFPy nanoplatform an promising candidate in biomedical clinical applications.

Novel three-dimensional fibrous covalent organic frameworks constructed via silver amalgam bridging for efficient organic dye adsorption and removal.

The construction of covalent organic frameworks (COFs) with unique structures has great significance in exploring the structure-function relationship and extending their potential applications. Fibrous COFs have demonstrated superior performance in specific application scenarios owing to the distinctive three-dimensional (3D) structure. Herein, we report a facile strategy for the fabrication of 3D COF nanofiber by exploiting silver amalgam as a bridging agent to assemble one-dimensional-extended PA-COF modules into a tubular structure. Dimensions of the obtained 3D COF nanofiber were predicted by DFT calculations, and the nanofiber was endowed with the merits of favorable uniformity and high stability. Due to the enhanced exposure of conjugatable binding sites for dye retention offered by the novel 3D architecture, the PA-COF nanofiber exhibits fast adsorption (within 5 min) and superior adsorption capacity to various organic dyes, e.g., 1717 mg g-1 for methylene blue (MB) and 978.3 mg g-1 for methyl orange (MO). Moreover, the PA-COF nanofiber shows excellent reusability in dye adsorption, which makes it a potential medium for removing dye pollutants from wastewater. This work presents an effective strategy to construct COF materials with unique architecture and potential prospects in the fields of separation and wastewater treatment.

Fabrication of P and N Co-Doped Carbon Dots for Fe3+ Detection in Serum and Lysosomal Tracking in Living Cells.

Doping with heteroatoms allows the retention of the general characteristics of carbon dots while allowing their physicochemical and photochemical properties to be effectively modulated. In this work, we report the preparation of ultrastable P and N co-doped carbon dots (PNCDs) that can be used for the highly selective detection of Fe3+ and the tracking of lysosomes in living cells. Fluorescent PNCDs were facilely prepared via a hydrothermal treatment of ethylenediamine and phytic acid, and they exhibited a high quantum yield of 22.0%. The strong coordination interaction between the phosphorus groups of PNCDs and Fe3+ rendered them efficient probes for use in selective Fe3+ detection, with a detection limit of 0.39 µM, and we demonstrated their practicability by accurately detecting the Fe3+ contents in bio-samples. At the same time, PNCDs exhibited high lysosomal location specificity in different cell lines due to surface lipophilic amino groups, and real-time tracking of the lysosome morphology in HeLa cells was achieved. The present work suggests that the fabrication of heteroatom-doped CDs might be an effective strategy to provide promising tools for cytology, such as organelle tracking.

Photoreversible DNA nanoswitch-based eluent-free strategy for the direct and effective isolation of highly-active thrombin from whole blood.

This study proposes an eluent-free isolation strategy for the direct isolation of thrombin from whole blood via tandem temperature/pH dual-responsive polyether sulfone monolith and photoreversible DNA nanoswitch-functionalized metal-organic framework (MOF) aerogel. Temperature/pH dual-responsive microgel immobilized on polyether sulfone monolith was adopted to remove the matrix complexity of blood sample via size/charge screening effect. Photoreversible DNA nanoswitches, comprising thrombin aptamer, aptamer complementary ssDNA (cDNA) and the azobenzene-modified ssDNA (control DNA), were functionalized on MOF aerogel to offer efficient capturing of thrombin under irradiation of ultraviolet light (365 nm), driven by electrostatic and hydrogen bond interactions. The release of captured thrombin was easily achieved by changing the complementary behaviors of DNA strands via blue light (450 nm) irradiation. Thrombin with purity higher than 95 % can be directly obtained from whole blood using this tandem isolation procedure. Fibrin production and substrate chromogenic tests showed that the released thrombin possessed high biological activity. The photoreversible thrombin capturing-release strategy is merited with eluent-free, avoiding the loss of activity of thrombin in chemical circumstances and undesired dilution, providing a robust guarantee for subsequent application.

Rational synthesis of carbon dots with phosphate ester group for direct mapping of endogenous alkaline phosphatase and polarity monitoring in living cells.

Carbon dots (CDs) have been extensively employed in biomolecule imaging. However, the imaging of biological enzymes with CDs has not been reported, which greatly limits their application in biological imaging. Herein, for the first time, a new type of fluorescent CDs is elaborately designed to realize the direct mapping of alkaline phosphatase (ALP) in cells. The obtained phosphorus and nitrogen co-doped CDs (P, N-CDs) generate specific structures including xanthene oxide and phosphate ester, thereby enabling P, N-CDs to be exclusively cleaved by ALP without auxiliary media. The fluorescence intensity of P, N-CDs can be specifically turned on in the presence of ALP, making them powerful probes for sensitive sensing of ALP activity with a detection limit of 1.27 U·L-1. Meanwhile, P, N-CDs possessing electron deficiency structure fulfill sensitive responding to polarity variations. The excellent photo-bleaching resistance and biocompatibility of the P, N-CDs are taken for directly mapping the intracellular endogenous ALP via turned-on fluorescence imaging, as well as real-time monitoring the polarity fluctuation in cells through ratiometric fluorescence imaging. The present work offers a new way to design and synthesize functional CDs for direct imaging of intracellular enzymes.