Latest ArticlesTransforming 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.
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.
The visible-light-induced selective oxidation of ubiquitous C–H bonds into valuable C=O bonds under aerobic conditions is one of the most attractive approaches for the construction of carbonyl-containing molecules. In this work, two transition metal-containing Nb/W mixed-addendum POMs dimers with the formula of K2Na2H5[(Fe(H2O)4)3(P2W15Nb3O62)2]·24H2O (POM[Fe]) and K2Na3H4[(Cr(H2O)4)3(P2W15Nb3O62)2]·32H2O (POM[Cr]) have been synthesized and characterized by various analytical and spectral techniques. POM[Fe] was proved to be an efficient photocatalyst for benzylic C–H oxidation under visible light and using oxygen as an oxidant to produce the corresponding carbonyl complex in good yields. A plausible mechanism involving superoxide radical was proposed for the catalytic reaction. POM[Fe] showed good reusability in the recycling experiments. IR spectroscopy and XRD analysis indicate that POM[Fe] can retain its integrity after catalysis.
Electrocatalytic oxygen evolution reaction (OER) is one of the important half reactions of electrocatalytic water splitting. However, the slow kinetic process involving four-electron transfer severely limits its reaction efficiency, which in turn limits the overall electrocatalytic hydrolysis efficiency. In order to improve the activity of the electrocatalytic OER, researchers mainly update the catalyst from three aspects, that is, increase the conductivity of the electrocatalyst, and the quantity and quality of active sites. Two-dimensional (2D) engineering can effectively reduce the resistance of the materials and greatly increase the number of electrochemically active sites, while heterometal doping, or the bimetal strategy, can improve the quality of active sites via changing the electronic structure of the material. Thus, the combination of the two can enhance the activity of electrocatalytic OER in all three aspects: conductivity, number and quality of active sites. However, there is currently no review on this topic. Therefore, in this review, we summarize the application of bimetallic 2D materials in electrocatalytic OER from four aspects: the structure, synthesis strategy, catalytic efficiency, and reaction mechanism.
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.
The first-principles calculations demonstrate that covalently bonded (cb) heterojunction and van der Waals (vdW) heterojunction can coexist in silicene/CeO2 heterojunctions, due to the different stacking patterns. Especially, the cb heterojunction with band gap of 1.97 eV, forms a type-II heterojunction, exhibits good redox performance and has high-effective optical absorption spectra, thus it is a promising photocatalyst for overall water splitting. Besides, for the vdW heterojunction, the Dirac cone of silicene is well kept on CeO2 semiconducting substrate, with a considerable energy gap of 0.43 eV, which can be an ideal material in building silicene-based electronic device. These results may open a new gateway in both of nanoelectronic device and energy conversion for silicene/CeO2 nanocomposites.
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.
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.
As an important anode material for fast-charging Li-ion batteries (LIBs), black phosphorus (BP) has attracted extensive attention. Black phosphorene nanotubes (BPNTs) can be theoretically produced by rolling up the black phosphorene nanosheet along armchair (a-BPNTs) and zigzag (z-BPNTs) directions. The effects of curvature, chirality, Li-storage concentrations and strain stress on the Li-storage performance such as Li diffusion barriers and mechanical stabilities of BPNTs are mainly investigated by first principles calculations. The theoretical calculations predict that the a-BPNTs and z-BPNTs have good maximum Li-storage capacities, and the z-BPNTs exhibit better flexibility than a-BPNTs. The mechanical stabilities and Li-migration are all related to the curvature of BPNTs. Additionally, both a-BPNTs and z-BPNTs exhibit fast Li-ion conductivity along the c-axis direction. Moreover, the average Poisson's ratio of a-BPNTs (0.68) is larger than that of z-BPNTs (0.17), indicating that the strain stress is more difficult to apply on a-BPNTs than z-BPNTs. Our calculations predict that the a-BPNTs can afford ultrafast kinetic rate for fast-charging and high-power LIBs, while the z-BPNTs can provide extra capacity for high-energy LIBs.
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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