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The first series of metal phosphate iodates, namely, M(IO3)(HPO4)(H2O) (M = Sc 1, Fe 2, Ga 3, In 4), have been obtained through hydrothermal syntheses. The title compounds are isomorphic and crystallize in the monoclinic space group C2/c (No. 15). Their structures feature a three-dimensional (3D) network composed of 1D [M(HPO4)(H2O)]+ chains that are further bridged by IO3 groups, forming 1D tunnels based on eight-membered rings along the b-axis. Magnetic measurements revealed antiferromagnetic coupling interactions between magnetic centers in compound 2. The UV absorption spectra measurements revealed that compound 2 exhibits a broad absorption peak at about 427 nm. The TGA studies and IR spectra for compounds 1–4 were also performed.
Herein, we introduce a facile approach to synthesize a unique class of Pt-M (M = Ni, Co) catalysts with a nanoflower structure for boosting both oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR). By controlling the surface-active agents, we modified the functional groups surrounding the Pt atoms, tuned the alloying of Pt and the transition metals Ni and Co, and prepared two different kinds of nanodendrites. Their successful synthesis depends on the selection and amount of surfactants (hexadecyltrimethylammonium bromide (CTAB), Polyvinylpyrrolidone (PVP)). Besides, by controlling reaction time, we also explored the forming procedures for Pt-Co globularia nanodendrite (Pt-Co GND) and Pt-Ni petalody nanodendrite (Pt-Ni PND). Our investigation highlights the importance of complex nanoarchitecture, which enables surface and interface modification to achieve excellent catalytic performance in fuel cell electrocatalysis. The characterization of the as-prepared catalysts reveals a high electrochemical surface area and mass activity (2041 m A m g P t - 1 and 950 m A m g P t - 1 for Pt-Co GND and Pt-Ni PND, respectively, for ORR). Furthermore, Pt-Co GND showed a high MOR activity, with a mass activity value recorded at 1615 m A m g P t - 1 which is far superior to that for Pt/C. Moreover, both catalysts retain high activity after accelerated durability tests (ADTs). The electron transfer number was calculated by performing the rotating ring-disk electrode (RRDE) measurements. Due to abundant active sites of Pt, both Pt-Co GND and Pt-Ni PND exhibit a 4e − pathway for ORR with electron transfer number of >3.95.
Abstract A series of metal-modified hierarchical M/H-ZSM-5 catalysts were prepared for catalytic conversion of cellulose in an aqueous medium. Characterization of the catalysts showed that the impregnation of metal into H-ZSM-5 did not change the basic framework and pore structure of H-ZSM-5, but it decreased the total acidity. Analysis of the products indicated that the catalysts significantly affected products distribution. When Co/H-ZSM-5 and Fe/H-ZSM-5 were used as the catalysts, the yields of lactic acid and cyclic ketones obviously increased. At last, a recommendable catalytic transformation pathway of cellulose over M/H-ZSM-5 was proposed on the basis of the obtained experimental results and the published literatures. Graphical Abstract In this paper, a series of metal-modified hierarchical M/H-ZSM-5 (M = Ce, Co, Ga, and Fe) catalysts were prepared and employed in catalytic conversion of cellulose in aqueous media to examined the products distribution of cellulose catalytic conversion. Based on our results and previous works, the plausible general reaction pathways of cellulose over M/H-ZSM-5 were proposed.
Glioblastoma (GBM) is a deadly brain tumor characterized by signaling dysregulation and aberrant cell cycle control. The CDK4/6-Rb axis is dysregulated in approximately 80% of all GBM cases. In this study, the anti-GBM effect of a novel pyrimidin-2-amine, LH20 was evaluated in vitro using the primary GBM cell lines U87MG and U251. GBM cells were administered LH20 at concentrations of 0.1, 1, 4, 8, 10, 20, 100, and 200 µM for 24 and 48 h, and the proliferation rate was evaluated using a CCK8 assay. Migration, apoptosis, and cell cycle were also assessed using a wound healing assay, Annexin V-FITC/PI apoptosis assay, and cell cycle staining, respectively. The targets of LH20 were predicted using SwissTargetPrediction and molecular docking. Western blotting analysis was performed to confirm the anti-GBM mechanism of LH20. We found that at concentrations of 4, 8, and 10 µM, LH20 significantly inhibited the proliferation and migration of U87MG and U251 cells, induced late phase apoptosis, promoted tumor cell necrosis, and arrested the G2/M phase of the cell cycle. LH20 also inhibited CDK4 and CDK6 activities by decreasing the phosphorylation of Rb. Our results suggest LH20 as a potential treatment strategy against GBM.Keywords:LH20;glioblastoma;apoptosis;G2/M;mitochondrial;CDKs
Bacterial infections result in significant burdens on public health, especially with the increasing prevalence of antibiotic resistance owing to the overuse of antibiotics. The development of the next-generation nanoantibacterial materials as alternatives to antibiotics is urgently needed. Metal–organic frameworks (MOFs) have been emerging as promising antibacterial materials. However, the impact of metal centers on the properties and antibacterial activity of MOFs has not been clarified to date. In this work, five M-MOF nanomaterials (M = Fe, Co, Ni, Cu, Zn) are synthesized with 2-methylimidazole as an organic ligand. Subsequently, the minimum inhibitory concentration (MIC), minimum bactericidal concentration, and time-kill curves are studied to evaluate their antibacterial activity. In addition, the destruction of the bacterial cells after treatment with M-MOFs is observed via scanning electron microscopy. The experimental results demonstrate that the Co-MOF and Zn-MOF polyhedra exhibit optimal antibacterial activity. They can effectively inhibit the growth of both Gram-negative bacteria Escherichia coli and Gram-positive bacteria Staphylococcus aureus at a low concentration. On the other hand, the Fe-MOF irregular particles show the weakest antibacterial activity among five M-MOFs and the antibacterial activity of the Ni-MOF and Cu-MOF nanosheets are comparable to each other. The huge difference in antibacterial activity of M-MOFs is attributed to the difference in the shape and size, specific surface area, surface charge, ion release, and production of reactive oxygen species. Overall, this study clarifies the relationship between metal centers in M-MOFs and their antibacterial activity.
Electrocatalytic seawater splitting for generating H 2 has become one of the most promising methods. This study prepared M-NiSe/Ni 3 Se 2 (M = Co, Fe, Cd) electrocatalysts through a one-step hydrothermal selenification reaction. In alkaline seawater, the Co–NiSe/Ni 3 Se 2 electrode requires overpotentials of 273, 369, and 431 mV to drive current densities of 10, 50, and 100 mA cm −2 for oxygen evolution reaction (OER) process, respectively. Moreover, the Co–NiSe/Ni 3 Se 2 electrocatalyst needs only potential of 1.395 V to drive a current density of 10 mA cm −2 in the urea oxidation reaction (UOR) process. According to density functional theory result, the synergistic effect between the large H 2 O adsorption capacity of Co–NiSe and the superior electrical conductivity of Ni 3 Se 2 is a key factor for contributing to the superior performance of the Co–NiSe/Ni 3 Se 2 catalyst. This study conducted systematic doping comparison experiments on the NiSe/Ni 3 Se 2 system, providing authentic and reliable experimental support for the design of selenide electrocatalysts.
Based on the galvanic replacement reaction between Cu nanoparticles and noble metal ions, a simple and efficient strategy was developed for the preparation of supported Cu–M (M = Pt, Pd, Ru, Rh) bimetallic nanoparticles under intense ultrasonication irradiation at ambient environment. A series of Cu–M/TiO2 bimetal catalysts with controllable composition, metal particle size less than 2 nm and narrow size distribution were obtained, and characterized by transmission electron microscopy (TEM), high resolution transmission electron microscope (HRTEM) with scanning TEM (STEM) mode, energy-dispersive X-ray spectrometers (EDS), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), and ICP-AES analysis. It was demonstrated that most of the metal particles were present in the form of bimetallic state. The mechanism of this strategy was discussed. The resultant Cu–Pd/TiO2 was used to reduce nitrate at room temperature, and it exhibited extremely high activity.
Adsorption desulfurization is a potential new method for deep desulfurization of fuel oil. The development of adsorbents with high adsorption capacity and selectivity is the core of deep adsorption desulfurization. The adsorption behavior of thiophene in MCM-41 mesoporous materials modified by various metal ions was studied in order to understand the adsorption desulfurization process of molecular sieves. The Fe-, Co-, and Zn-modified MCM-41 materials were prepared using a one-step in situ hydrothermal synthesis method. The modified MCM-41 molecular sieves maintained the mesoporous structure, and the metal ions had specific dispersion on the surface of the molecular sieves. Adsorption of thiophene on the surfaces of molecular sieves had both physical and chemical characteristics. The adsorption desulfurization performance of the modified molecular sieve was superior to that of the pure silica molecular sieve. In the simulated gasoline with sulfur content of 220 μg/g, when the amount of adsorbent used was 100 mg, the adsorptive desulfurization performance tended to be in equilibrium, and the optimum adsorption temperature was 30°C. Fe-MCM-41 and MCM-41 molecular sieves reached adsorption equilibrium after ~60 min, but the desulfurization rate of Co-MCM-41 and Zn-MCM-41 still increased slightly. The kinetic simulation results indicated that the pseudo-second-order kinetics adsorption model described well the adsorption process of thiophene on molecular sieves. The molecular sieve Fe-MCM-41 had the best desulfurization performance with an equilibrium adsorption capacity of 14.02 mg/g and the desulfurization rate was ~90%.
Searching for low-cost electrocatalysts with high activity towards the hydrogen evolution reaction (HER) is of great significance to enable large-scale hydrogen production via water electrolysis . In this study, by using inverse spinel MFe 2 O 4 (M = Mn, Fe, Co, Cu) nanoparticles (NPs) as the precursors, monodisperse bimetallic phosphide M-Fe-P NPs/C with hollow structures were readily obtained by a gas-solid annealing method. These hollow phosphide NPs displayed excellent HER activity in an acidic medium with a low loading amount of 0.2 mg cm −2 . In particular, the Co–Fe–P NPs/C shows highest HER activity that only requiring an overpotential of 97 mV to retain a current density of 10 mA cm −2 . A volcano relation between activity and incorporated elements was revealed. Incorporation of cation with high electronegativity stabilized the FeP active centres, while phase segregation resulted in the loss of activity for Cu–Fe–P NPs/C.
According to relative energy band positions between noble metals of Au, Ag, and wide bandgap semiconductor SnO 2 , Au, and Ag nanoparticles (NPs) modified hollow SnO 2 NPs were designed. Firstly, the hollow SnO 2 NPs have been synthesized by employing the silica template-assisted hydrothermal methods, then Au and Ag were coated on the surface of SnO 2 to form the core–shell structures, respectively. The morphology, composition, and optical properties of as-prepared samples have been investigated by various analytic methods. Subsequently, the photocatalytic reaction to Rhodamine B (RhB) dye under simulated-sunlight irradiation was employed to investigate their photocatalytic performance, the results demonstrate the metal–semiconductor with direct Schottky contact exhibited remarkable photocatalytic activity . The finite difference time domain (FDTD) calculation results illustrate the introduced and decorated Au and Ag NPs could enhance the harvesting abilities for visible light. We envision the aforementioned synthesized strategy and catalytic results are used to the designing and application of other metal–semiconductor system.
Intermolecular energetic materials (IEMs) have become the focus of attention due to their excellent performance in combustion, ignition, energy release and sensitivity. In this paper, two IEMs were successfully designed and prepared by the self-assembly of 5-aminotetrazole (5-ATZ) and transition metal ions on the surface of ammonium perchlorate (AP) particles. The scanning electron microscope, infrared spectroscopy, powder X-ray diffraction, thermogravimetric analyses, and differential thermal analyses were employed to characterize the prepared samples. The results show that the surface of AP particles is completely covered by a uniform and dense M(5-ATZ) 4 Cl 2 (M = Cu, Co) self-assembled layer. Thermal analyses show that the high-temperature decomposition peak temperatures of AP/Cu(5-ATZ) 4 Cl 2 (10 wt%) and AP/Co(5-ATZ) 4 Cl 2 (10 wt%) are decreased by 93.3 °C and 127.1 °C compared to the case of pure AP, while the heat releases of them are increased by 539 J∙g −1 and 580 J∙g −1 . In addition, the burning rates of AP/Cu(5-ATZ) 4 Cl 2 /Al (10 wt%) and AP/Co(5-ATZ) 4 Cl 2 /Al (10 wt%) are increased by 6.8 mm∙s −1 and 7.8 mm∙s −1 compared with the case of AP/Al. Moreover, the hygroscopicity tests show that the prepared samples do not agglomerate aftter being placed in the atmosphere with a relative humidity of 79% for 66 h. This research shows considerable application prospects in improving the combustion and energy performance of solid propellants, it is also a reference for the design and preparation of other novel IEMs.
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