Latest ArticlesThe development of high-performance non-precious metal-based robust bifunctional electrocatalyst for both hydrogen evolution reaction (HER) and oxygen evolution reactions (OER) in alkaline media is essential for the electrochemical overall water splitting technologies. Herein, we demonstrate that the HER/OER performance of CoSe2 can be significantly enhanced by tuning the 3d-orbital electron filling degree through Mo doping. Both density functional theory (DFT) calculations and experimental results imply that the doping of Mo with higher proportion of the unoccupied d-orbital (Pun) could not only serve as the active center for water adsorption to enhance the water molecule activation, but also modulate the electronic structures of Co metal center leading to the optimized adsorption strength of *H. As expected, the obtained Mo-CoSe2 exhibits a remarkable bifunctional performance with overpotential of only 85 mV for HER and 245 mV for OER to achieve the current density of 10 mA/cm2 in alkaline media. This work will provide a valuable insight to design highly efficient bifunctional electrocatalyst towards HER and OER.
Through uncomplicated carbonation process, a carbon-embedded CoNiSe2/C nanosphere was synthesized from Ni-Co-MOF (metal-organic framework) precursor whose controllable structure and synergistic effect of bimetallic Ni/Co brought CoNiSe2/C anodes with high specific surface area (172.79 m2/g) and outstanding electrochemical performance. CoNiSe2/C anodes obtained reversible discharge capacities of 850.9 mAh/g at 0.1 A/g after cycling for 100 cycles. In addition, CoNiSe2/C exhibits excellent cycle stability and reversibility in the rate test at a current density of 0.1–2.0 A/g. When the current density returns to 0.5 A/g for 150 cycles, its discharge ratio the capacity is 330.8 mAh/g. Electrochemical impedance spectroscopy (EIS) tests suggested that CoNiSe2/C anodes had a lower charge transfer impedance of 130.02 Ω after 30 cycles. In-situ X-ray diffraction (XRD) tests confirmed the alloying mechanism of CoNiSe2/C which realized higher lithium storage capacity. This work affords substantial evidence for the extension of bimetallic selenides in secondary batteries, promoting the development of bimetallic selenides in anode materials for LIBs.
The emission changes of fluorescent dyes under the influence of environmental changes or interaction with analytes are the basis for designing ratiometric fluorescent probes and logic gates. However, it is rare that only one external stimulus induces continuous fluorescent color changes in a fluorescent dye. In this paper, we report a cage-like molecule formed by two benzene rings and three imidazolium salts which produces continuous fluorescence wavelength changes when interacted with fluoride ions. Fluoride ions are first bound to the center of the cage under the action of anion-π interaction, and the (C−H)+···F– type ionic hydrogen bonds induce the blue-shift of fluorescence. The subsequent formation of C-F covalent bonds with fluoride ions makes the fluorophore wavelength continue to blue-shift, and finally obtains continuous multiple fluorescence changes caused by a single external stimulus. According to the fluorescence wavelength and intensity, six different fluorescence signal channels can be obtained, which can be encoded as six numbers from 0 to 5. We expect that this reaction process can find applications in quantitative anion recognition and molecular counters.
The hydroarylation reaction of terminal alkynes with arylboronic acids catalyzed by low (400 ppm) loadings of palladium has been developed. The reaction is broad in scope and high-yielding, even on multi-gram scale. It is suitable for the synthesis of alkenes labeled with deuterium, and for the late-stage modification of bioactive molecules.
Coordination-driven self-assembly was used to construct two metallacycles of a dicarboxylate-functionalized dibenzo-18-crown-6 in combination with either a 0° anthracene-based clip-type acceptor or a 60° phenanthrene-based acceptor. The angularities of these moieties make them suitable for the formation of a [2 + 2] rectangle and a [3 + 3] triangle, respectively. The synthesis, characterization and host-guest chemistry of two metallacycles were described and supported by 31P{1H}, 1H NMR spectra and electrospray mass spectrometry.
Decades have passed since the first nanoparticles-base medicine was approved for human cancer treatment, and the research and development of nanoparticles for drug delivery are always undergoing. Nowadays, the significant advances complicate nanoparticles' branches, including liposomes, solid lipid nanoparticles, inorganic nanoparticles, micelles, nanovaccines and nano-antibodies, etc. These nanoparticles show numerous capabilities in treatment and diagnosis of stubborn diseases like cancer and neurodegenerative diseases, emerging as novel drug carriers or therapeutic agents in future. In this review, the complicated branches of nanoparticles are classified and summarized, with their property and functions concluded. Besides, there are also some delivery strategies that make nanoparticles smarter and more efficient in drug delivery, and frontiers in these strategies are also summarized in this review. Except these excellent works in newly-produced drug delivery nanoparticles, some points of view and future expectations are made in the end.
The development of deep-red emitting lead-free metal-halide perovskites with high photoluminescence quantum yields (PLQYs) and outstanding stability remains a major challenge for displays and deep-tissue bioimaging. In this work, we report a facile and convenient solvothermal method to synthesize metal halides Cs2ZnX4 (X = Cl, Br) that however is PL innert at room temperature. Upon composition engineering utilizing Sn2+ as the dopant, the resulting Cs2ZnCl4: Sn not only emits strong deep-red PL peaked at 700 nm with the highest 99.4% PLQY among the similar materials so far, but also exhibits excellent structure stability in air (PLQY remains 96% after one year exposure to the atmosphere). Detailed experimental characterizations and theoretical calculations reveal that the deep-red emission stems from self-trapped excitons induced by the Sn2+ dopant. Particularly, triplet emission (3P2→1S0) from Sn-5s2 orbitals has been observed at low temperature due to the break of parity-forbidden transition. This work provides an important guidance for the development of deep-red light-emitting materials with low price, high efficiency and excellent stability.
An efficient palladium-catalyzed electrooxidation C–H acylation reaction of N-nitrosoanilines with α-oxocarboxylic acids was developed. The anodic oxidation of the Pd(Ⅱ) intermediate was found to be the key to complete the reaction. In this case, the N-nitroso group was observed to be an effective directing group for C–H activation reaction. Moreover, the synthetic transformation of derivatives of natural products (L-menthol, dehydroepiandrosterone, and pregnenolone) was successfully realized. Finally, flow electrochemical synthesis of some substrates was achieved.
G-quadruplex (G4) is widely known as a non-classical secondary structure of nucleic acid. With the in-depth study of G4, it is an urgent need for a phosphorescent probe with a high G4 binding ability to evaluate the level of G4 in the cytoplasm. Thus, this study designed and synthesized Ir-PDP where an Ir(Ⅲ) complex was used as a phosphorescent emitter. Meanwhile, two installed PDPs (pyridostatin derivatives) were used to improve the combination ability with G4 and reduced the cytotoxicity of the Ir(Ⅲ) complex. Compared with other nucleic acid secondary structures, Ir-PDP produced a higher phosphorescence lifetime after interacting with G4. Ir-PDP was distributed in the cytoplasm of living cells, and two-photon phosphorescence lifetime imaging can detect the binding events of the probe in the cytoplasm. The addition of G4 binder PDS significantly regulated cytoplasmic phosphorescence lifetime. The project explored a new sensing pathway to observe the binding manners of probes in the cytoplasm through the phosphorescence lifetime of probes.
Cu2-xS nanostructures have been intensively studied as outstanding chemodynamic therapy (CDT) and good photothermal therapy (PTT) antibacterial agents due to their highly efficient Cu(Ⅰ)-initiated Fenton-like catalytic activity and good photothermal conversion property. However, they still suffer from shortage of Cu(Ⅰ) supply in the long-term and comparatively low inherent photothermal conversion efficiency. Herein, we constructed a self-enhanced synergistic PTT/CDT nanoplatform (Cu1.94S@MPN) by coating Cu1.94S nanoparticles with Fe(Ⅲ)/tannic acid based metal-polyphenol networks (MPN). Activated by the acidic bacterial infection microenvironment, Cu1.94S@MPN could be decomposed to continuously release Cu(Ⅱ), Fe(Ⅲ) ions and tannic acid. As the result of tannic acid-involved Cu and Fe redox cycling, Cu(Ⅰ)/Fe(Ⅱ)-rich CDT could be achieved through the highly accelerated catalytic Fenton/Fenton-like reactions. More importantly, experimental results demonstrated that Cu1.94S@MPN exhibited both excellent photothermal antibacterial and photothermal-enhanced CDT properties to eradicate bacteria in vitro and in vivo. Overall, this novel nanotherapeutics has great potential to become a clinic candidate for anti-infective therapy in future.
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