Latest ArticlesAlthough targeted therapy and immunotherapy are now shining in the treatment of some cancers, chemotherapy is still the cornerstone of drug treatment for many cancer patients. The emergence of chemotherapy prodrugs can improve the drug activity and reduce the side effects of chemotherapy. When used, the tumor microenvironment has characteristics different from normal tissues, and the existence of the microenvironment provided a more convenient way to design responsive nanodrugs. Herein, we designed a glutathione (GSH)-responsive prodrug nanogels for enhancing tumor chemotherapy. In the nanogels of HHNP, 10-hydroxycamptothecin (HCPT) played an essential role in killing cancer cells. HCPT was jointed with a cross-linker agent with disulfide bond and was further coated with polyethylene glycol, which not only prolonged the half-life of the drug, but also made HCPT accurate transport to the tumor fractions and achieved precise and controllable release. The proposal of HHNP effectively retained the biological activity of the drug, and introduced functions such as targeting, selective release and biodegradation, which greatly improved the medical efficiency of the drug and effectively reduced the toxic and side effects. This chemotherapeutic prodrug nanogel offers a new window for constructing efficient drug delivery platform.
To 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.
A new, stable and scalable reagent for deuteriodifluoromethylthiolation (deuterated N-difluoromethylthiophthalimide, PhthSCF2D) has been developed. This reagent can be applied for the photocatalytic radical deuteriodifluoromethylthiolation of various olefins and aldehydes (30 examples). Meanwhile, it can achieve the electrophilic deuteriodifluoromethylthiolation of a series of electrophilic substrates including electron-rich arenes, aryl/vinylboronicacids, alkynes, amines, thiols and β-ketoesters (22 examples). Some complex molecules can also be applied in both radical and electrophilic deuteriodifluoromethylthiolation using PhthSCF2D as the reagent.
Two unprecedented polycyclic spirooliganones C and D (1 and 2) with a novel spiro[bicyclo[2.2.2]octane-2, 2′-bicyclo[3.1.0]hexane] carbon skeleton, one known dimeric prenylated C6C3 compound (3), and a pair of new enantiomeric prenylated C6C3 compounds (+)-5 and (−)-5 together with their direct precursors (+)-4 and (−)-4 were isolated from the roots of Illicium oligandrum. Their structures and absolute configurations were elucidated by spectroscopic analysis, single crystal X-ray diffraction data, and electronic circular dichroism calculations. A possible biosynthetic pathway for compounds 1 and 2 involving the Diels-Alder reaction between (−)-sabinene and cyclic prenylated tetrahydropyrano-type C6C3 compounds was proposed. The characteristic prenylated C6C3 compounds (+)-4 and (−)-4 were separated on a chiral stationary phase and their absolute configurations were determined by calculated ECD for the first time. In the antiviral bioassays, compounds 1 and (+)-5 exhibited significant inhibitory activity against CVB3 with IC50 values of 11.11 µmol/L and 1.11 µmol/L, respectively. Compounds 1 and 2 also showed moderate inhibition against influenza A (H1N1) virus.
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.
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.
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.
Corneal wound closure for surgical eye surgeries or accidents is typically performed to prevent pathogens from the sterile intraocular environment and avoid potential postoperative complications. Tissue adhesives are increasingly employed for corneal wound closure with superior treatment efficiency and less adverse effects. In this study, we successfully develop a novel corneal adhesive based on functionally coupled PEG-lysozyme (PEG-LZ) hydrogels for wound closure after surgical eye surgeries. PEG-LZ hydrogels have plenty of micropores and gradually decreased pore size with increasing concentration from 10%, 15% to 20% (w/v), in which PEG-LZ (15%) represents the suitable pH value, gelation time and elastic modulus. PEG-LZ hydrogels have no in vitro cytotoxicity and excellent ex vivo wound closure effectiveness in porcine eyes. The in vivo wound sealant in rabbit eyes by PEG-LZ hydrogels presents a superior therapeutic effect compared with the conventional methods of stromal hydration and suture, in terms of the wound closure percent, mean corneal thickness, percent of wound gaping, and the Descemet membrane detachment. PEG-LZ hydrogels do not induce obvious histological pathology changes. The PEG-LZ corneal adhesive is considered as a tissue adhesive alternative for wound closure after surgical eye surgeries.
Relying on the electron energy loss spectrum (EELS) of metallic elements to obtain microstructure analysis is an investigation method of the reaction mechanisms of transition metal oxides (TMOs) in catalysis, energy storage and conversion. However, the low signal from K shell owing to insufficient electron beam energy, and the complicated electronic structure in L shell of the metal element restrict the analysis of the coordination environment of the TMOs. Herein, density functional theory (DFT) calculation, Fourier transform (FT) and wavelet transform (WT) were employed to probe the relationship between the four individual peaks in O K-edge spectra of iron oxides and the microstructure information (chemical bonds and atomic coordination). The findings show that the peak amplitude ration is in a linear correlation with the valence state of Fe element, and that the coordination number obtained by radial distribution function (RDF) is favorably linearly correlative with that from the standard coordination structure model. As a result, the quantitative analysis on the change of valence state and atomic coordination in microstructure can be realized by EELS O K-edge spectra. This study establishes EELS O K-edge spectrum as a promising pathway to quantitatively analyze the valence state and atomic coordination information of TMOs, and offers an effective method to conduct microstructure analysis via the EELS spectra of the non-metal element.
As an extensively applied therapeutic approach to combat tumors, radiotherapy generates localized ionizing radiation to destruct tumor cells. Despite its importance in clinical oncology, radiotherapy would often cause significant organ toxicity, and its therapeutic effect is limited by tumor hypoxia. Moreover, although abscopal therapeutic effects have occasionally been observed, radiotherapy is still mostly employed as a local treatment method that could hardly control tumor metastases. In recent years, strategies involving biomaterials and nanomedicine have received increasingly high attention to enhance cancer radiotherapy. Beyond sensitizing tumors for radiotherapy via various mechanisms, many biomaterial systems with immune stimulating effects have also been introduced to boost the antitumor immunity post cancer radiotherapy. In this mini-review, we will summarize the progress of different biomaterials and nanomedicine systems in combination with radiotherapy to trigger antitumor immune responses and enhance the efficacy of immunotherapy, and discusses the perspectives and challenges of this research direction aimed at clinical translations.
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