Latest ArticlesPhotosensitization related to energy/electron transfer process is of great importance to natural photosynthesis. Herein, we proposed a promising strategy to improve the sensitizing ability of the typical photoactive MOFs (UiO-Ir) by engineering its metal coordination center with NBI (1, 8-naphthalenebenzimidizole) chromophore. The resulting MOFs (UiO-Ir-NBI) exhibited a strong sensitizing ability for significantly boosting photosynthesis. Impressively, the catalytic yield of 2-chloroethyl ethyl sulfoxide with UiO-Ir-NBI can reach 99%, over 6 times higher than that with UiO-Ir (16.4%). Moreover, UiO-Ir-NBI exhibited an excellent catalytic stability and a broad substrate tolerance, highlighting its great application prospect. Systematic investigations revealed that the strong visible light absorption, long excited state lifetime and efficient electron-hole separation of UiO-Ir-NBI greatly contributed to harvesting visible light and facilitating interface electron/energy transfer for efficient solar energy utilization. This work provides a new horizon to boost photosythesis of MOFs by engineering their metal sensitizing centers at a molecular level.
In the face of multiple challenges brought by the changes of global climate and environment, developing clean energy and updating green energy storage equipment are important ways to achieve carbon peak and carbon neutrality. Aqueous batteries have become a research hotspot due to their advantages of using the multivalent charge carrier, high ionic conductivity, environmental friendliness and cost effectiveness. In this work, the Cu2Se@C (Cu2Se coated on carbon clothes) thin film with a three-dimensional braided structure is fabricated by a simple electrochemical deposition method for Cu2+ storage for the first time. Compared with the commercial Cu2Se powder, the well-designed Cu2Se@C film shows enhanced specific capacity (640 mAh/g at 0.5 A/g) and rate performance (542 mAh/g at 5 A/g) as well as superior cycling stability (82.7% capacity retention after 1000 cycles at 1 A/g). The Cu2+ storage mechanism of the Cu2Se@C electrode is based on a reversible phase transition process of Cu2Se ↔ Cu2-xSe ↔ CuSe ↔ CuSe2. In kinetic characteristic analysis, the Cu2Se@C electrode demonstrates faster Cu2+ diffusion in discharge process than charge process resulting from the phase transition and the variation of interplanar spacing. This work highlights a facile one-piece design strategy and opens a new gateway for the exploration of advanced aqueous energy storage systems.
Nanoplastics (NPs) in aqueous environment have become a category of emerging pollutants on account of their potential risks to both human health and environment. The detection of NPs is a great challenge due to the lack of sensitive and selective sensing materials with fast response time and wide sensing range of particle sizes. Herein, a Tb-based coordination polymer has been synthesized for luminescent detection of nanopolystyrene with different particle sizes in aqueous solutions, showing a low limit of detection, fast response time within 10 s and high selectivity in the presence of other plastics. The “turn-on” sensing mechanism is studied in detail. This work provides a facile method for the fast detection of NPs.
The present study reported fabrication of novel carbon quantum dots-MnFe2O4@ZIF-8 (CQDs-MFO@ZIF-8) by using co-precipitation hydrothermal method for activation of peroxydisulfate (PDS) to degrade bisphenol A (BPA), one of important emerging organic pollutants in water environment. CQDs-MFO@ZIF-8 served as a highly efficient thermal activated PDS catalyst with high catalytic degradation efficiency, reusability and stability. The catalyst achieved almost completely removal of 20.0 mg/L BPA within 5.0 min, and the degradation efficiency remained higher than 83% after 5 consecutive cycles. Free radicals (•OH, SO4•− and •O2−) and non-free radicals (1O2) were generated in the thermal PDS-activation system, in which singlet oxygen (1O2) played a dominant role in the degradation of BPA. The potential toxicity of BPA degradation intermediates was analyzed upon the culture of E. coli and Chlorella sorokiniana by using Ecological Structure-Activity Relationship Model (ECOSAR) program. The catalytic performances of BPA degradation by CQDs-MFO@ZIF-8 were evaluated for treatment of different practical water samples to further verify the feasibility of practical applications. This study provides proof-in-concept demonstration of new nanomaterials for enhanced catalytic water decontamination.
Herein, we report the facile synthesis of a highly strained hexabenzocoronene-containing carbon nanoring, cyclo[4]-paraphenylene[2]-2,11-hexabenzocoronenylene ([4,2]CPHBC), as the segment of a [10,10] single-walled carbon nanotube ([10,10]SWNT). [4,2]CPHBC was synthesized based on the platinum-mediated assembly of diborylbiphenyl and diborylhexabenzocoronene, forming a tetranuclear platinum complex, followed by reductive elimination. This nanoring molecule was confirmed by NMR and HR-MS, and its photophysical properties were studied using steady-state and time-resolved spectroscopies. Moreover, the selective supramolecular host-guest interaction between [4,2]CPHBC and C60 was also investigated.
Glioblastoma multiforme (GBM) is the most common malignant primary brain tumor in adults. The precise identification and distinction of GBM heterogeneity from surrounding brain parenchyma at the cellular level and even at the tissue level are important for GBM therapy. In this study, GBM cells are distinguished from normal astrocytes and non-central nervous system (CNS) tumor cells by surface-enhanced Raman scattering (SERS) based on gold nanoshell (SiO2@Au) particles and support vector machine (SVM) algorithm. In addition, the gold nanoisland (AuNI) SERS substrates are further developed and explored for accurate detection of GBM at the tissue level. The distinction between glioma and trauma tissues, identification of different tumor grades, and IDH mutation are realized with the assistance of orthogonal partial least squares discriminant analysis (OPLS-DA) in a rapid, non-invasive, and convenient method. The results show that the developed SERS-based analytical method has the potential for practical application for the detection of GBM at the single-cell and tissue levels and even for real-time intraoperative diagnosis.
Sulfydryl-contained (-SH) substances including hydrogen sulfide (H2S), cysteine (Cys), homocysteine (Hcy) and glutathione (GSH) play crucial roles in living systems, and their variations are closely associated with various diseases. Herein, we developed a near-infrared intramolecular charge transfer (ICT) based fluorescent probe Y-NBD, achieving detection of Cys/Hcy and H2S with different fluorescent signals (green-red for Cys/Hcy, red for H2S), large Stokes shifts (~100/105 nm or 191 nm) and high signal-background-ratio, but not responding to GSH. Y-NBD was successfully applied to image exogenous/endogenous Cys/Hcy and H2S in various living cancer cells (HeLa, A549, and HepG2) and in zebrafish. It not only visualized the transformation pathway of several thiols in HepG2 cells but also verified that the intestine is the main site for the activation and metabolism of Y-NBD in zebrafish, as well as realized to evaluate the degree of drug-induced liver injury. This work provides a promising tool for imaging Cys/Hcy and H2S in living systems and shows great potency in evaluating drug-induced liver injury and its treatment.
Molecular recognition in water, the biological solvent, always receives significant research focus in supramolecular chemistry. The mechanisms of molecular recognition in water is key to comprehending biological processes at the molecular level. Over the past five decades, supramolecular chemists have developed a vast array of synthetic receptors with highly diverse structures and recognition properties. Among them, cyclophanes represent an important family of macrocyclic receptors that have been extensively explored. The aromatic moieties in cyclophanes not only facilitate chemical modifications to impart water solubility but also enable forming hydrophobic cavities for guest inclusion in aqueous environments. Pioneered by Koga et al., who reported the first inclusion complex of cyclophanes in water and solid state, numerous water-soluble cyclophanes, including derivatives of blue box, calixarenes, resorcinarenes, pillararenes, octopusarenes, biphenarenes, coronarenes, and naphthotubes, etc., have been synthesized and subjected to investigation of the recognition capabilities in aqueous solutions. This review provides an overview of cyclophane receptors designed to bind organic guests in water. We categorize them into two classes based on the modifications made to their hydrophobic cavities: those with "exo-functionalized hydrophobic cavities" and those with "endo-functionalized hydrophobic cavities". We introduce their distinctive features and discuss strategies to enhance recognition affinity and selectivity. This review aims to inspire the development of novel synthetic receptors with intriguing properties and foster practical applications of cyclophanes.
The galactomannan from Antrodia cinnamomea (AC) is characterized as one of the important bioactive components that exhibits potential immunostimulatory propriety. The biological function of its corresponding oligosaccharide fragments has not been revealed yet. In this study, we reported the first chemical synthesis of the series of oligosaccharide fragments related to AC galactomannan via the convergent glycosylation strategy. The preliminary immunological evaluation of these synthesized AC oligosaccharides disclosed that the backbone tetrasaccharide 1d showed the best immunomodulatory ability on enhancing proliferation, phagocytosis and cytokines secretion of Raw264.7 macrophages in vitro, indicating its immense potential as an immunostimulant candidate.
As key biomarkers, amyloid-β (Aβ) plaques are frequently used to diagnose Alzheimer's disease (AD). Although fluorescence imaging has proven to be effective in detecting these plaques, the gold standard probe thioflavin T (ThT), used for Aβ aggregates, cannot be applied in vivo owing to its invasive nature. Therefore, the development of novel fluorescent probes capable of identifying Aβ plaques in situ is necessary. Based on the ThT structure, two π-conjugated heterocyclic D-π-A probes were designed bearing the hydroxytricyanopyrrole acceptor and N,N-dimethylaminophenyl donor. These probes exhibited red to near-infrared fluorescence emission (λmax = 732 nm), large Stokes shifts (>100 nm), exceptional signal-to-noise ratio, rapid response (<30 s), and high binding affinity (NT-HTCP = 33.32 nmol/L; NF-HTCP = 53.35 nmol/L) for Aβ aggregates. As the best candidate, NT-HTCP was used for in situ imaging of Aβ plaques in AD mouse models. Furthermore, in vivo research demonstrated that NT-HTCP could cross the blood–brain barrier and continue imaging the Aβ plaques with a good signal-to-noise ratio. Additionally, the outcomes of the docking computations helped guide the development of the Aβ probes. This study expands the family of N,N-dimethylaminophenyl-based Aβ-sensitive fluorophores, with NT-HTCP emerging as a highly promising imaging agent.
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