Latest ArticlesTo develop efficient concerted companion (CC) dyes for fabricating high-performance DSSCs, three organic dyes XL1-XL3 have been designed by varying the position and number of the β-hexylthiophene (HT) bridges, and these organic dye units are covalently linked with our previously reported porphyrin dye XW10 to construct the corresponding CC dyes XW74-XW76. Among the organic dyes, XL3 contains two β-hexylthiophene units at both the donor and acceptor parts and thus possesses stronger light-harvesting capability in the green light region. Because of the most complementary absorption between XL3 and XW10 as well as the excellent photovoltaic behavior of the individual XL3 dye, the corresponding CC dye XW76 affords the best PCE (10.78%) among all the CC dyes. Upon coadsorption with CDCA, XW76 affords a highest PCE of 11.35%, which outperforms the previous cosensitization system of XW10+WS-5. This work provides an approach for developing efficient DSSCs based on CC dyes composed of an organic dye unit with suitable π spacers inserted at appropriate positions.
Stabilizing triplet excited states is important for room temperature phosphorescence (RTP) materials to achieve multifunctional applications in humid environment. However, due to the lack of preparation strategies, the realization of RTP materials in water still faces challenges. Herein, a new design strategy was presented to achieve RTP in water by confining carbonized polymer dots (CPDs) in amino functional mesoporous silica (MSNs-NH2). The as-prepared MSNs-CPDs aqueous dispersion exhibited blue afterglow, lasting more than 3 s to naked eyes. The triplet excited states were protected from non-radiative deactivation by the double-confinement effect including covalent bonding fixation and mesoporous structure confinement. The MSNs-CPDs inherited the structure of MSNs-NH2, so the stability of morphology and properties were superior to CPDs and even most of silica-based CPDs RTP materials. A water-related encryption technique demonstrated the promising application of MSNs-CPDs as smart materials in the field of information security. Besides, the possibility of potential application in ion detection was also explored.
Available online The abnormal carboxylesterase (CES) expression is closely related to many diseases such as hyperlipidemia, atherosclerosis, obesity, liver cancer, type 2 diabetes mellitus and gastrointestinal stromal tumors. The detection of a single enzyme in practical samples is often constrained by the structural diversity of CESs. Thus, the development of broad-carboxylesterase responsive fluorescent probe, which can detect the presence of wide variety of CESs, may provide overall or category information from another point of view, supplementing the deficiency of single detection for CES subspecies. Organelle lysosome is involved in various cell processes, such as cell signaling, apoptosis, secretion, and energy metabolism. Up to date, lysosome-targeted fluorescent probes, especially those with red emission (over 550 nm, with relatively low biological harmfulness), for CES detection are still rare. A lysosomes-targeted red fluorescent probe CES-Lyso was designed to monitor intracellular a variety of carboxylesterases alteration with wonderful selectivity and sensitivity, which was further applied to distinguish different derived breast cancer cells and monitor carboxylesterase activity in the anticancer drug treatment.
Since the concept of aptamer emerged, many scientists have launched a rich field of research around it. However, few nucleic acids aptamer which use cell as target can be put into practical applications. We believe that a great deal of this lies in the complexity and irreproducibility of aptamer screening experiments themselves. The complexity is due to the cumbersome processes and the technical requirements for laboratory personnel, whereas irreproducibility arises from the fact that the starting point of such screens is nucleic acid libraries with random fragments, and that different libraries directly determine the differences or even the success or failure of screening results. The complexity and irreproducibility mentioned above, in turn, lead to the inability of this experiment to unfold on a large scale, which naturally cannot lead to excellent results for practical applications. In response to this problem, our group has developed an instrument for automated screening of tumor cell nucleic acid aptamers and characterized the properties of nucleic acid aptamers obtained using this instrument in a comprehensive manner.
Selective cleavage of robust C−C bonds to harvest value-added aromatic oxygenates is an intriguing but challenging task in lignin depolymerization. Photocatalysis is a promising technology with the advantages of mild reaction conditions and strong sustainability. Herein, we show a novel urchin-like Nb2O5 hollow microsphere (U-Nb2O5 HM), prepared by one-pot hydrothermal method, are highly active and selective for Cα−Cβ bond cleavage of lignin β-O-4 model compounds under mild conditions, achieving 94% substrate conversion and 96% C−C bond cleavage selectivity. Systematic experimental studies and density functional theory (DFT) calculations revealed that the superior performance of U-Nb2O5 HMs arises from more exposed active sites, more efficient free charge separation and the active (001) facet, which facilitates the activation of Cβ−H bond of lignin models and generate key Cβ radical intermediates by photogenerated holes, further inducing the Cα−Cβ bond cleavage to produce aromatic oxygenates. This work could provide some suggestions for the fabrication of hierarchical photocatalysts in the lignin depolymerization system.
In this paper, three new polyoxometalates (POM)-based metal–organic complexes constructed from a new semi-rigid organic ligand N,N'-bis(4-pyrimidinecarboxamido)-1,2-cyclohexane (4-bpmah) H2[Cu(4-bpmah)2(SiMo12O40)(H2O)2]·2H2O (1), H[Cu(4-bpmah)2(PMo12O40)(H2O)2]·2H2O (2) and [Cu(4-bpmah)(H2O)2]·[Cu2(TeMo6O24)(H2O)10]·4H2O (3) were synthesized by hydrothermal method. Single crystal X-ray analyses showed that complexes 1 and 2 were isostructural, in which the isolated Keggin-type [SiMo12O40]4–/[PMo12O40]3– anions and [Cu(4-bpmah)2(H2O)2]2n+ units were expanded into 3D supramolecular structures through hydrogen bond interactions. In complex 3, the 1D [Cu(4-bpmah)(H2O)2]2n+ metal–organic chains and isolated [Cu2(TeMo6O24)(H2O)10]2n– units were expanded into a 3D supramolecular framework by the hydrogen bond interactions. In this paper, carbon cloth working electrodes composited by the title complexes (1/CC, 2/CC and 3/CC) were prepared and used as electrodes for supercapacitors. The performance of supercapacitors as well as the influence of electrolyte solution and title complexes quality load on the performance of supercapacitors were studied. Furthermore, the electrochemistry and electrocatalytic behaviors of complexes 1–3 bulk-modified carbon paste electrodes (1-CPE, 2-CPE and 3-CPE) toward the reduction of KBrO3, KNO2, Cr(Ⅵ), as well as their sensing behaviors on Cr(Ⅵ) were investigated.
The development of a single analytical platform with different functions is highly desirable but remains a challenge at present. Here, a paper-based device based on fluorescent carbon dots (CDs) functionalized paper/MnO2 nanosheets (MnO2 NS) hybrid devices (PCD/NS) was proposed for single-device multi-function applications. MnO2 NS functioned as a fluorescence quencher of CDs and recognizer of H2O2 released from the oxidase catalyzed system. Fluorescence recovery would occur after the decomposition of MnO2 NS induced by H2O2, by which a simple and effective strategy could be developed for fluorescence monitoring multiplex biological events. Xanthine (XA) sensing, xanthine oxidase (XOD) inhibitors screening analysis and chiral recognition of glucose enantiomers were performed on PCD/NS to investigate the multifunctional application of the paper-based device. By means of PCD/NS, XA could be determined in the range of 0.1–40 µmol/L with a low detection of limit of 0.06 µmol/L. The IC50 value of allopurinol, the model inhibitor of XOD, was sensitively detected to be 7.4 µmol/L. Glucose enantiomers were also recognized in terms of the specific fluorescence response to d-glucose. This work firstly presented a paper-based device capable of biomarkers detection, inhibitors screening and chiral recognition, which enlightened a promising strategy for the construction of multifunctional devices and hold the great potential application in clinical diagnosis and drug discovery.
Two pairs of fluorescent natural products, talarolactones (+)/(−)-A and (+)/(−)-C [(+)/(−)-1 and (+)/(−)-2], were discovered and characterized as a new family of circularly polarized luminescence-active small organic molecules (CPL-SOMs) with high fluorescence efficiency and fascinating CPL properties. The CPL (|glum|) levels of enantiomerically pure (+)/(−)-1 and (+)/(−)-2 in solution falls into the usual range (10−5−10−3) considering their pure organic nature, but the sign of CPL were found to be closely related to the absolute configuration of C-8. The high agreement of the measured CPL spectra of (+)/(−)-1 and (+)/(−)-2 with the time-dependent density functional theory (TDDFT) calculated ones demonstrated the usefulness of CPL-calculation as a unique method for stereochemical assignment. This study may open up a new perspective for the stereochemical studies and the future development of CPL materials.
A series of near-infrared (NIR) fluorescent substrates (NDRO-1~8) derived from fluorophore NDRH with different volumes of ester bond as the recognition group were designed and synthesized for the detection of acetylcholinesterase (AChE), among which NDRO-1 with the smallest acetate group displayed the highest activity toward AChE. The detection limit of NDRO-1 for sensing AChE was 0.32 µg/mL, and Km was 6.40 µmol/L, indicating ultra-sensitivity and good affinity of NDRO-1 toward AChE. NDRO-1 was used to detect the inhibitory of four kinds of pesticides including methamidophos, dichlorvos, and the detection limit was lower than 50 µg/L, which was further used in pesticide residues detection.
The BiOCl (BOC) synthesized by the water bath heating method was treated with sodium borohydride (NaBH4) to introduce oxygen vacancies (OVs). At the same time, Au nanoparticles were loaded to prepare a series of Au/BiOCl samples with different ratios. OVs and Au nanoparticles can promote the light absorption of host photocatalyst in the visible region. The calculated work function of BiOCl and Au can verify the existence of Ohmic contact between the interface of them, which is conducive to the separation of charge carriers. Through a series of photoelectric tests, it was verified experimentally that the separation of charge carriers is indeed enhanced. The high-energy hot electrons produced by Au under the surface plasmon resonance (SPR) effect can increase the counts of electrons to participate in the CO2 reduction reaction. Especially for 1.0%-Au/BOC, the yields of CO can reach 43.16 µmol g−1 h−1, which is 6.6 times more than that of BOC. Therefore, loading precious metal on semiconductors is an effective strategy to promote the photocatalytic performance of CO2 reduction reactions.
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