Latest ArticlesNanoscale metal organic frameworks (NMOFs) have been widely reported in biomedical field for their unique porous structure and tunable multifunctionality. However, when administrated in vivo, the protein corona will be formed on the surface of NMOFs, significantly affecting their biodistribution, pharmacokinetics and drug release. Few studies paid attention to the protein corona formation process and its influencing factors of NMOFs. As a well-established strategy for altering structure features of NMOFs, the organic ligand modification may have effect on the protein corona formation process, which is to be investigated. In this study, the zirconium (Zr)-based UIO66 was chosen as model NMOFs, the organic ligand of which was modified with amino group (-NH2) or carboxyl group (-COOH) to synthesize UIO66-NH2 and UIO66-2COOH, respectively. Bovine serum albumin (BSA) was chosen as model protein to investigate the protein corona formation process of NMOFs. The current results showed that the -COOH modification remarkably enhanced the BSA adsorption on NMOFs while -NH2 slightly decreased the protein binding affinity. These differences may be ascribed to the two different dominate protein corona formation modes, i.e., surface coating mode and porous embedded mode. The protein corona formation did not affect the crystal phase of NMOFs but increased the content of α-helix of BSA. Ultimately, upon protein corona formation, the cellular uptake of NMOFs was significantly affected. We believe our study will provide a new research paradigm to the design and applications of NMOFs.
A catalytic asymmetric hydroxylative dearomatization reaction has been disclosed, and the products can smoothly transform into spiroannulation adducts by simply treated with a base under mild conditions. Novel in-situ generated magnesium catalytic methods are developed by application of combinational ligands. Related concise transformaitons of the spiroannulation adducts have been carried out.
Transforming immature DCs into mature state to activate cellular immunity is a critical step in initiating immunoprophylaxis and immunotherapy. Lipopolysaccharides (LPS) can promote DCs maturation by binding receptor on DCs surface, but their clinical application is limited due to biological toxicity. Although many LPS analogues have been developed, complex synthesis and purification hinder their practical application. Here, we propose a novel and simple strategy to synthesize LPS analogues with adjustable structural units. Using monomer units similar to the key functional groups of LPS, we synthesize LPS analogues with different group ratios by RAFT polymerization. The obtained analogues have little negative effect on cell viability. Compared with LPS, the analogues show greater promoting effect on DCs maturation. And the analogues can be applied to different scenarios since the degrees of promoting DCs maturation by LPS analogues with different group ratios are different. This strategy provides a new direction for synthesizing LPS analogues, and it has the potential to produce LPS analogues on a large scale with tunable promoting DCs maturation effect.
Selective hydrogenation of cinnamaldehyde (CAL) toward cinnamyl alcohol (COL) is an extremely important and challenging reaction. Herein, a series of PtxFey-Al2O3 bimetallic catalysts with varied Pt to Fe ratios were prepared by incipient wetness impregnation method. The introduction of Fe significantly modifies the electronic and surface properties of Pt, which clearly enhances the C=O hydrogenation selectivity. Among all the catalysts, Pt3Fe-Al2O3 displays the best catalytic performance and the conversion of CAL is 96.6% with 77.2% selectivity of COL within 1 h. In addition, Pt3Fe-Al2O3 had excellent reusability with 76% COL selectivity after five runs of the recycle process. Further characterization of the fresh, used and cycled catalysts revealed that the structure and electronic state of the synthesized PtxFey-Al2O3 are unchanged after hydrogenation reaction. The identical-location transmission electron microscopy (IL-TEM) results revealed that the interaction between the nanoparticles and the supports was strong and the catalyst was relatively stable.
Surface-enhanced Raman scattering (SERS) spectroscopy has been employed as a rapid analysis technology for food security inspection recently. Nowadays, it is still a great challenge to rapidly quantify multiple trace antibiotics potentially abused in aquaculture industry. In this work, a magnetic Ti3C2Tx/Fe3O4/Ag substrate was prepared for the development of a reliable rapid SERS quantification method for multiple trace sulfonamides in aquatic products. This magnetic substrate had good uniformity, reproducibility, stability and SERS activity. Moreover, this substrate could integrate the magnetic separation-enrichment and matrix clean-up without cross contamination, which endowed it with good selectivity and anti-interference capability during real sample analysis. The electromagnetic enhancement and chemical enhancement mechanism of this magnetic substrate were studied in detail to reveal its good separation-enrichment performance and SERS activity. Finally, a rapid SERS quantification method was established and practically applied for trace phthalic sulfathiazole (PST) and silver sulfadiazine (SSD) in aquatic products by using Ti3C2Tx/Fe3O4/Ag magnetic substrates. Trace PST and SSD could be actually detected and quantified as 55.9 µg/kg and 64.0 µg/kg in aquatic products, respectively. Good recoveries of 83.9%–116% with relative standard deviations (RSDs) of 0.5%–3.2% for PST and 80.2%–102% with RSDs of 1.3%–5.8% for SSD were obtained. This work proposed an efficient and reliable method for rapid quantification of trace multiple sulfonamides in complex aquatic samples during food security inspection.
Quasi-two-dimensional (q2D) conducting polymer thin film synergizes the advantageous features of long-range molecular ordering and high intrinsic conductivity, which are promising for flexible thin film-based micro-supercapacitors (MSCs). Herein, we present the high-performance flexible MSCs based on highly ordered quasi-two-dimensional polyaniline (q2D-PANI) thin film using surfactant monolayer assisted interfacial synthesis (SMAIS). Owing to high electrical conductivity, rich redox chemistry, and thin-film morphology, the q2D-PANI MSCs show high volumetric specific capacitance (ca. 360 F/cm3) and energy density (17.9 mWh/cm3), which outperform the state-of-art PANI thin-film based MSCs and promise for future flexible electronics.
The lithium dendrite growth is still a serious challenge and impeding the realistic applications of all-solid-state lithium batteries. In view of the amide containing sediment layer can be stable on lithium/cathodes, a composite polymer electrolyte with amide-based matrix is in-situ built on porous electrodes. With the introduction of amide, the polymer electrolyte presents excellent ability to inhibit lithium dendrite growth and makes the Li/Li symmetric battery stably work for 500 h with a good ionic conductivity of 4.25 × 10−5 S/cm at 40 ℃. The solid electrolyte also shows a wide electrochemical stable window and good interface contact with the porous cathode. Utilizing this composite polymer electrolyte, the all-solid-state Li/LiFePO4 battery shows an initial discharge capacity of 146.5 mAh/g at 0.1 C under 40 ℃ and remains 81.4% in 100 cycles. The polymer electrolyte also can present better properties after modification. These results demonstrate that the presented PA-based composite polymer electrolyte could be served as a good electrolyte candidate for all-solid-state lithium-ion batteries.
Iron fluoride (FeF3) is considered as a promising cathode material for Li-ion batteries (LIBs) due to its high theoretical capacity (712 mAh/g) with a 3e− transfer. Herein, we have designed a strategy of hierarchical and mesoporous FeF3/rGO hybrids for LIBs, where the hollow FeF3 nanospheres are the main contributor to the specific capacity and the 2D rGO nanosheets are the matrix elevating the electronic conductivity and buffering the volume expansion. The unique FeF3/rGO hybrid can be rationally synthesized by a non-aqueous in-situ precipitation method, offering the merits of large specific surface area with rich active sites, fast transport channels for lithium ions, effective alleviation of volume expansion during cycles, and accelerating the electrochemical reaction kinetics. The FeF3/rGO hybrid electrode possesses a high initial discharge capacity of 553.9 mAh/g at a rate of 0.5 C with 378 mAh/g after 100 cycles, acceptable rate capability with 168 mAh/g at 2 C, and feasible high-temperature operation (320 mAh/g at 70 ℃). The superior electrochemical behaviors presented here demonstrates that the FeF3/rGO hybrid is a potential electrode for LIBs, which may open up a new vision to design high-efficiency energy-storage devices such as LIBs based on transition metal fluorides.
Lithium–sulfur (Li–S) battery is labeled as a promising high-energy-density battery system, but some inherent drawbacks of sulfur cathode materials using relatively complicated techniques impair the practical applications. Herein, an integrated approach is proposed to fabricate the high-performance rGO/VS4/S cathode composites through a simple one-step solvothermal method, where nano sulfur and VS4 particles are uniformly distributed on the conductive rGO matrix. rGO and sulfiphilic VS4 provide electron transfer skeleton and physical/chemical anchor for soluble lithium polysulfides (LiPS). Meanwhile, VS4 could also act as an electrochemical mediator to efficiently enhance the utilization and reversible conversion of LiPS. Correspondingly, the rGO/VS4/S composites maintain a high reversible capacity of 969 mAh/g at 0.2 C after 100 cycles, with a capacity retention rate of 82.3%. The capacity fade rate could lower to 0.0374% per cycle at 1 C. Moreover, capacity still sustains 795 mAh/g after 100 cycles in the relatively high-sulfur-loading battery (6.5 mg/cm2). Thus, the suggested method in configuring the sulfur-based composites is demonstrated a simple and efficient strategy to construct the high-performance Li–S batteries.
Aqueous zinc energy storage devices, holding various merits such as high specific capacity and low costs, have attracted extensive attention in recent years. Nevertheless, Zn metal anodes still suffer from a short lifespan and low Coulombic efficiency due to corrosion and side reactions in aqueous electrolytes. In this paper, we construct an artificial Sn inorganic layer on Zn metal anode through a facile strategy of atom exchange. The Sn layer suppresses Zn dendrite growth by facilitating homogeneous Zn plating and stripping during charge and discharge processes. Meanwhile, the Sn protective layer also serves as a physical barrier to decrease Zn corrosion and hydrogen generation. As a result, The Sn-coated anode (Sn|Zn) exhibits a low polarization voltage (~34 mV at 0.5 mAh/cm2) after 800 testing hours and displays a smooth and an even surface without corrosion. Moreover, the zinc ion capacitor (Sn|Zn||activated carbon) is assembled with an enhanced capacity of 42 mAh/g and a capacity retention of 95% after 10,000 cycles at 5 A/g. This work demonstrates a feasible approach for the commercialization of aqueous Zn-based energy storage devices.
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