Latest ArticlesThe P2-type manganese-based Na0.7MnO2 cathode materials attract great interest due to their high theoretical capacity. However, these materials suffer from rapid capacity fading, poor rate performance and severe voltage decay resulting from phase transition and sluggish reaction kinetics. In this work we report a novel Nb-doped Na0.7[Ni0.3Co0.1Mn0.6]1-xNbxO2 with significantly suppressed voltage decay and enhanced cycling stability. The strong Nb-O bond can efficiently stabilize the TMO framework, and the as prepared material demonstrates much lower discharge midpoint voltage decay (0.132 V) than that of pristine one (0.319 V) after 200 cycles. Consequently, a remarkably improved cycling performance with a capacity retention of 87.9% after 200 cycle at 0.5 C is achieved, showing a 2.4 fold improvement as compared to the control sample Na0.7Ni0.3Co0.1Mn0.6O2 (~37% rotation). Even at 2 C, a capacity retention of 68.4% is retained after 500 cycles. Remarkably, the as prepared material can be applied at low temperature of −20 ℃, showing a capacity retention of 81% as compared to that at room temperature.
The recent boom in large-scale energy storage system promotes the development of lithium-oxygen batteries because of their high theoretical energy density. However, their applications are still limited by the sluggish kinetic, insoluble discharge product deposition and the undesired parasitic reaction. Herein, the free-standing nitrogen doped reduced graphene oxide/Co(OH)2 (NRGO/Co(OH)2) composite films were prepared by a facile hydrothermal method. The NRGO/Co(OH)2 composite films display interconnected three-dimensional conductive network, which can not only promote the diffusion of O2 and the transport of electrolyte ions, but also provide abundant storage space for discharge products. Moreover, the introduction of nitrogen-containing functional groups results in improved conductivity and electron adsorption ability, which can facilitate electron transport and enhance the surface catalytic activity. Combining with excellent catalytic performance, the lithium-oxygen batteries with NRGO/Co(OH)2 composite film cathodes deliver low charge overpotential and excellent cycling performance.
Hydrous electrolytes with high electrochemical potentials were obtained by hydrating water molecules into solutes to form high Li: water molar ratio electrolytes (HMRE). Solid polyethylene glycol (PEG) were employed to enhance the molar ratio of Li+ to water in the electrolytes while reducing the consumption of Li-salt. The obtained mole ratio of Li+ to water molecules in the hydrous electrolytes was greater than 1:1; however, the mass fraction of Li-salt was reduced to 61% (approximately 5.5 mol/kg, based on water and PEG). Compared with that of water-in-salt electrolytes, the mass fraction of Li-salt could be remarkably reduced by adding solid PEG. The electrochemical stability of the electrolytes improved considerably because of the strong hydration of Li+ by the water molecules. A beneficial passivation effect, arising from the decomposition of the electrolyte, at a wide potential window was observed.
The design of pore structure is the key factor for the performance of porous carbon spheres. In this work, novel micron-sized colloidal crystal microspheres consisting of fibrous silica (F-SiO2) nanoparticles are firstly prepared by water-evaporation-induced self-assembly of F-SiO2 nanoparticles in the droplets of an inverse emulsion system to be used as sacrificial templates. Acrylonitrile (AN) was infiltrated in the voids of the F-SiO2 colloidal crystal microspheres, and in-situ induced by 60Co γ-ray to polymerize into polyacrylonitrile (PAN). After the PAN-infiltrated F-SiO2 colloidal crystal microspheres were carbonized and etched with HF solution, novel micron-sized inverse-opal N-doped carbon (IO-NC) microspheres consisting of hollow carbon nanoparticles with a hierarchical macro/meso-porous inner surface were obtained. The IO-NC microspheres have a specific surface area as high as 266.4 m2/g and a molar ratio of C/N of 5. They have a good dispersibility in water, and show a high adsorption capacity towards rhodamine B (RhB) up to 137.28 mg/(g microsphere). This work offers a way to obtain novel micron-sized hierarchical macro/meso-porous N-doped carbon microspheres, which opens a new idea to prepare high-performance hierarchical porous carbon materials.
Herein, we directly prepared white fluorescent CDs (W-CDs) using 1,6-dihydroxynaphthalene (1,6-DHN) and L-asparagine (L-Asn) as carbon sources through a simple solvent-free method. As-prepared W-CDs can be obtained in high yield (95%). A relative pure white LEDs (WLEDs) were fabricated with Commission Internationale de L'Eclairage (CIE) coordinates of (0.32, 0.31). As-prepared W-CDs will have promising future for a wide range of optoelectronic devices.
Amorphous silicon (a-Si) is one of the most promising anode-materials for the lithium-ion battery owing to its large capacity and superior fracture resistance. However, a-Si is usually fabricated with the sophisticated chemical vapor deposition or pulse laser deposition in a limited scale. In this work, we have successfully prepared a-Si spheres (~200 nm) by reducing the TiO2-coated silica spheres with Al powders in the molten salts at 300 ℃. The coated TiO2 layer acts as a protective layer for structural maintenance during the reduction and a precursor for doping. The doped Ti element may suppress the crystal growth of Si to facilitate the formation of a-Si. The observation with in-situ transmission electron microscopy (TEM) further reveals that lithiation kinetics of the synthesized a-Si is controlled by the interfacial reaction. The Li+ diffusivity in a-Si determined from the observation is in the order of 10−14 cm2/s. The anode of a-Si spheres together with crystalline Si nanoparticles exhibits excellent electrochemical performance, delivering a reversible capacity of 1604 mAh/g at 4 A/g and a capacity retention of 78.3% after 500 cycles. The low temperature reduction process reported in this study provides a low-cost method to fabricate a-Si nanostructures as high-capacity durable anode materials
The development of high-performance and cost-effective electrocatalysts towards oxygen reduction reaction (ORR) is of significant importance, but still challenging for the practical applications in related energy systems. ORR process typically suffers from sluggish kinetics, the exploration of ORR electrocatalyst thus requires elaborate design. Herein, an effective strategy is developed for growing Co/N-doped carbon nanotube arrays on 2D MOFs-derived matrix via the pyrolysis of Co/Zn metal-organic-framework (MOF) nanosheets. The Co/Zn-MOF nanosheets serve as both the self-template for the 2D carbonized framework morphology and C/N source for the in-situ growth of 1D N-doped carbon nanotubes. The constructed hierarchical architecture effectively integrates the 0D/1D Co nanoparticle/N-doped carbon nanotube interface and 1D (nanotubes)/2D (nanosheets) junction into frameworks with highly exposed active surface, enhanced mass-transport kinetics and electrical conductivity. As a result, the designed composite exhibits superior ORR activity and durability in alkaline media as compared to commercial Pt/C. Particularly, it shows promising ORR performance with a half-wave potential of 0.78 V versus reversible hydrogen electrode and negligible activity attenuation after 5000 potential cycles in acidic electrolyte. The designed strategy can be extended to construct other MOFs-derived carbon matrixes with diverse hierarchical structures and provide an efficient avenue for searching high-performance electrocatalysts.
Circulating tumor DNA (ctDNA) refers to a class of acellular nucleic acids carrying genetic features of primary tumor, which can be regarded as a promising noninvasive biomarker for cancer diagnosis. The development of ctDNA assay is an important component of liquid biopsy. In this study, we have fabricated a novel electrochemical strategy for ultrasensitive detection of ctDNA combining the merits of strand displacement amplification and DNA nanostructures. Stable DNA triangular prism is firstly self-assembled and modified on the electrode surface. After target initiated strand displacement polymerization reaction, the generated DNA product helps the formation of three-way junction nanostructure on triangular prism, which localizes electrochemical species. By carefully investigating the electrochemical responses, the limit of detection (LOD) for ctDNA assay as low as 48 amol/L is achieved. This proposed electrochemical biosensor shows great potential for clinical applications.
Nanoarchitectonics provide versatile opportunities for modifying the properties of coordination polymers (CP) other than molecular engineering. Spatial-controlled etching focuses on the controlled disassembly of the frameworks. The etching method provides an excellent opportunity for tailoring the properties and functions of the CPs. Here, we discuss the mechanism for controlled etching of the CPs and summarized the two main strategies utilized so far. Several examples are illustrated to demonstrate recent developments in this area. Moreover, advantages of the etched CPs are summarized in several important applications, including energy storage, catalysis and nanomedicine.
Pincer complexes are widely used in organometallic and coordination chemistry. The role of antimony as a central donor atom in pincer ligands has been extensively explored in recent years. Although phenylenediamine derived PXP (X = B, Al, C, Si, Ge, Sn, N) type ligands exhibit diverse reactivity, analogues species based on antimony have been reported less frequently. Herein, we report a new PSbP complex and evaluate its reactivity. These species will broaden the family of phenylenediamine derived pincer complexes.
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