Latest ArticlesMetal-organic frameworks (MOFs) are a class of outstanding materials in Li-air batteries because of their high surface areas, tailorable pore sizes and diverse catalytic centers. However, MOF-based batteries are facing challenges such as poor electronic conductivity and inferior long-cycle stability that limit their further development. This review first summarizes the progress of pristine MOFs and MOF-derived materials in Li-air batteries in the past 5 years, then provides a perspective for subsequent development of MOFs and their derivatives in this emerging field.
Bimetallic nanoparticles (AmBn) usually exhibit rich catalytic chemistry and have drawn tremendous attention in heterogeneous catalysis. However, challenged by the huge configuration space, the understanding toward their composition and distribution of A/B element is known little at the atomic level, which hinders the rational synthesis. Herein, we develop an on-the-fly training strategy combing the machine learning model (SchNet) with the genetic algorithm (GA) search technique, which achieve the fast and accurate energy prediction of complex bimetallic clusters at the DFT level. Taking the 38-atom PtmAu38-m nanoparticle as example, the element distribution identification problem and the stability trend as a function of Pt/Au composition is quantitatively resolved. Specifically, results show that on the Pt-rich cluster Au atoms prefer to occupy the low-coordinated surface corner sites and form patch-like surface segregation patterns, while for the Au-rich ones Pt atoms tend to site in the core region and form the core-shell (Pt@Au) configuration. The thermodynamically most stable PtmAu38-m cluster is Pt6Au32, with all the core-region sites occupied by Pt, rationalized by the stronger Pt-Pt bond in comparison with Pt-Au and Au-Au bonds. This work exemplifies the potent application of rapid global search enabled by machine learning in exploring the high-dimensional configuration space of bimetallic nanocatalysts.
In this paper we report the desgin and synthesis of dihydroxyindoles oligomers based reversible fluorescence sensor. We find dihydroxyindoles-2-carboxylic acid derived oligmer (P-DHICA) has the highest selectivity and sensitivity for Cu2+ detection. This work provide a highly efficient, environmentally friendly biosensor for potential use in medical testing.
Nitrogen photofixation using g-C3N4-based photocatalysts have attracted abundant of attentions recently. Herein, in this study, holey g-C3N4 (HGCN) nanosheets possess a good deal of carbon vacancies were prepared by means of thermally treating bulk g-C3N4 (BGCN) under an NH3 atmosphere. Characterization analysis revealed that the as-synthesized sample have identical crystal structure, larger BET specific surface area, stronger reduction capability, and higher photogenerated charge carrier separation rate than that of BGCN. These properties may contribute to enhance the nitrogen photofixation activity. It was also found that the rate of NH4+ production for N2 photofixation of HGCN sample reached~25.54 mg L-1 h-1 gcat-1, which is approximately~5.87 times higher than that of BGCN sample under optimal reactive conditions. Moreover, a plausible mechanism of HGCN for nitrogen photofixation process was illuminated in detail.
Antimony-based materials have become promising anodes within lithium-ion batteries (LIBs) due to their low cost and the high theoretical capacity. However, there is a potential to further enhance the electrochemical performance of such antimony-based materials. Herein, Sb2Se3@C nanofibers (Sb2Se3@CNFs) are designed and obtained via a novel electrospinning method. Upon electrochemically testing as an anode within LIBs, the Sb2Se3@CNFs (annealed at 600 ℃) delivers a remarkably good cycling performance of 625 mAh/g at 100 mA/g after 100 cycles. Moreover, it still remains at 490 mAh/g after 500 cycles with an applied current density of 1.0 A/g. The excellent performance of the Sb2Se3@CNFs can be attributed to the fact that the N-doped C matrices not only remit the volume expansion of materials, but also enhance the electrical and ionic conductivity thusly increasing the lithium-ion diffusion. The obtained Sb2Se3@CNFs are promising anode for LIBs in the future.
Several novel pyridine-oxadiazole iridium complexes were synthesized and characterized through X-ray crystallography. The designed iridium complexes revealed surprisingly high catalytic activity in C-N bondformation of amides and benzyl alcohols with the assistance of non-coordinating anions. In an attempt to achieve borrowing hydrogen reactions of amides with benzyl alcohols, N, N'-(phenylmethylene)dibenzamide products were unexpectedly isolated under non-coordinating anion conditions, whereas N-benzylbenzamide products were achieved in the absence of non-coordinating anions. The mechanism explorations excluded the possibility of "silver effect" (silver-assisted or bimetallic catalysis) and revealed that the reactivity of iridium catalyst was varied by non-coordinating anions. This work provided a convenient and useful methodology that allowed the iridium complex to be a chemoselective catalyst and demonstrated the first example of non-coordinating-anion-tuned selective C-N bond formation.
A series of novel phenylpyrazole carboxylic acid derivatives containing fluorine moiety, i.e., diamides 11, simple aryl-bearing amides 12 and acylthioureas 14 were successfully synthesized based on the key fluoro-containing phenylpyrazole acid intermediate. The new compounds were identified and confirmed by melting point, 1H NMR, 13C NMR and elemental analysis or HRMS. The bioassay results indicated that some of the compounds possessed excellent insecticidal activities towards oriental armyworm, diamondback moth and corn borer at low concentrations. For examples, compounds 11a, 11e-g and 14b exhibited remarkable larvicidal activities with LC50 values of 0.13-0.39 mg/L and 0.0002-0.0014 mg/L against oriental armyworm and diamondback moth, respectively, were comparable with those of the control chlorantraniliprole. Particularly, 11e were found superior to chlorantraniliprole in oriental armyworm tests (LC50:0.23 mg/L vs. 0.26 mg/L); 11a, 11e, 11f and 14c in diamondback moth tests with LC50 values of 0.0002 mg/L, 0.0002 mg/L, 0.0008 mg/L and 0.0005 mg/L, respectively, were more effective than that of chlorantraniliprole. In addition, 12a also showed a promising insecticidal potential and development/optimization advantage. Compounds 11a, 11e-g, 12a, 14b and 14c could be considered as possible new leading structures for further study. The SAR investigation indicated that the compounds with fluorine motif (e.g., -F, -CF2H, -CF3) held apparently favorable insecticidal potentials, which provided useful guidance for further design/development of new phenylpyrazole-containing agrochemicals.
β-Elemene is a volatile oil used for the treatment of cancer, but poor solubility, low bioavailability, and various adverse reactions limit its application. For ameliorating risks of the venous toxicity of β-elemene, intravenously injectable micelle of β-elemene was prepared using the thin-film hydration method. The results pointed out the micelles were uniformly spherical with about 20.96 ± 0.1966 nm in average diameter and exhibited high entrapment efficiency (99.02% ± 0.88%). As revealed by drug release studies in vitro, β-elemene micelles had sustained drug release. Compared with free β-elemene, the micelles increased the drug cellular uptake and enhanced the anti-tumor effect in vitro through retarding cell cycle and inducing apoptosis. Meanwhile, the elevated serum stability of β-elemene micelles implied less drug leakage and reduced toxicity. The wound healing and tube formation assay in vitro demonstrated the anti-metastasis and anti-angiogenesis effects of β-elemene micelles. Moreover, the pharmacokinetics study showed the AUC and T1/2 of β-elemene in micelle group were 1.79 and 1.62 times of that in free β-elemene group, suggesting the circulation time of β-elemene in the blood had been prolonged. In addition, β-elemene micelles showed a favorable antitumor response compared with the β-elemene solution on C26 colon cancer-bearing mice model. Local irritation study investigated in rabbits indicated that the β-elemene micelles strikingly mitigated the irritation to the injection sites compared with free β-elemene. These results proved that the micelle could be a good candidate as an auspicious drug delivery system of β-elemene for the prospective clinical treatment of carcinoma.
Spirooxindoles play an important role in drug discovery and development. The development of efficient methods for the synthesis of spirooxindoles from easily available starting materials is of current interest. Herein, we report in detail the In(OTf)3-catalyzed [3 + 3] annulation of spirocyclopropyl oxindoles and 1, 4-di-thiane-2, 5-diol, which allows the facile preparation of spiro[indoline-3, 4'-thiopyran]-2-ones bearing (tetrahydro)thiopyran skeleton.
In this work, we adopt a new tobramycin (TOB)-dopamine coating system to endow thin film composite membranes with excellent antifouling and antimicrobial properties. Combining the hydrophilic and antibiofouling properties of both TOB and polydopamine, the TOB-dopamine modified membrane exhibits improved antifouling and antimicrobial properties compared with the conventional dopamine modified and unmodified membranes. The TOB-dopamine system has two advantages over the conventional modification with dopamine and tris buffer solution. First, TOB-dopamine modification is more efficient than the conventional dopamine modification due to the accelerating effect of TOB on dopamine polymerization. Second, the TOB-dopamine modified membranes exhibit better hydrophilicity, and enhanced antifouling and antimicrobial properties than the conventional dopamine modified membrane. Beyond engineering membranes, the proposed TOB-dopamine system can also be extended for wider surface hydrophilic and antimicrobial modifications.
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