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1.
Inorg Chem ; 2020 Apr 23.
Artigo em Inglês | MEDLINE | ID: mdl-32323981

RESUMO

Transition metal phosphides (TMPs) have gained increased attention in energy storage due to their potential applications for optimizing electrochemical performances. However, their preparation routes usually require highly toxic and flammable phosphorus sources with strict reaction conditions. The existence of multiple energetically favorable stoichiometries also makes it a challenge to achieve phase control of metal phosphides. In this work, we have successfully realized the phase-controllable framework of cobalt phosphide from Co2P to CoP by employing a semi-interpenetrating network (semi-IPN) hydrogel as a precursor. Interestingly, the semi-IPN hydrogel could serve as a self-assembly/sacrificing template to accomplish 3D space confinement, where poly(vinylphosphonic acid) (PVPA) was identified as a prominent phosphorus source due to its strong metal complexation ability and high thermal stability. Furthermore, this route is successfully extended to the synthesis of other TMPs, including Fe2P, Ni2P, and Cu3P. The specific structure of cobalt phosphides gives rise to superior lithium storage performance, showing superior cycling stability (495.2 mAh g-1 after 1000 cycles at 2.0 A g-1). This approach envisions a new outlook on exploitation of essential functional hydrogels for the creation of inorganic materials toward sustainable energy development.

2.
Adv Sci (Weinh) ; 5(7): 1800241, 2018 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-30027054

RESUMO

Hierarchical nanoscale carbons have received wide interest as electrode materials for energy storage and conversion due to their fast mass transfer processes, outstanding electronic conductivity, and high stability. Here, heteroatom (S, P, and N) doped hierarchical vesicular carbon (HHVC) materials with a high surface area up to 867.5 m2 g-1 are successfully prepared using a surface polymerization of hexachloro-cyclotriphosphazene (HCCP) and 4,4'-sulfonyldiphenol (BPS) on the ZIF-8 polyhedrons. Significantly, it is the first time to achieve a controllability of the wall thickness for this unique carbon, ranging from 18 to 52 nm. When utilized as anodes for sodium ion batteries, these novel carbon materials exhibit a high specific capacity of 327.2 mAh g-1 at 100 mA g-1 after 100 cycles, which can be attributed to the expanded interlayer distance and enhanced conductivity derived from the doping of heteroatoms. Importantly, a high capacity of 142.6 mAh g-1 can be obtained even at a high current density of 5 A g-1, assigning to fast ion/electronic transmission processes stemming from the unique hierarchical vesicular structure. This work offers a new route for the fabrication/preparation of multi-heteroatom doped hierarchical vesicular materials.

3.
Adv Sci (Weinh) ; 5(6): 1800080, 2018 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-29938187

RESUMO

Different dimensions of carbon materials with various features have captured numerous interests due to their applications on the tremendous fields. Restricted by the raw materials and devices, the controlling of their morphology is a major challenge. Utilizing the catalytic features of the intermediates from the low-cost salts and polymerization of 0D carbon quantum dots (CQDs), 0D CQDs are expected to self-assemble into 1/2/3D carbon structures with the assistance of temperature-induced intermediates (e.g., ZnO, Ni, and Cu) from the salts (ZnCl2, NiCl2, and CuCl). The formation mechanisms are illustrated as follows: 1) the "orient induction" to evoke "vine style" growth mechanism of ZnO; 2) the "dissolution-precipitation" of Ni; and 3) the "surface adsorption self-limited" of Cu. Subsequently, the degree of graphitization, interlayer distance, and special surface area are investigated in detail. 1D structure from 700 °C as anode displays a high Na-storage capacity of 301.2 mAh g-1 at 0.1 A g-1 after 200 cycles and 107 mAh g-1 at 5.0 A g-1 after 5000 cycles. Quantitative kinetics analysis confirms the fundamentals of the enhanced rate capacity and the potential region of Na-insertion/extraction. This elaborate work opens up an avenue toward the design of carbon with multidimensions and in-depth understanding of their sodium-storage features.

4.
Analyst ; 141(8): 2542-52, 2016 Apr 21.
Artigo em Inglês | MEDLINE | ID: mdl-27027375

RESUMO

Techniques of isothermal amplification have recently made great strides, and have generated significant interest in the field of point-of-care detection. Nicking endonuclease-mediated isothermal amplification (NEMA) is an example of simple isothermal technology. In this paper, a real-time quantitative nicking endonuclease-mediated isothermal amplification with small molecular beacons (SMB-NEMA) of improved specificity and sensitivity is described. First, we optimized the prohibition of de novo synthesis by choosing Nt·BstNBI endonuclease. Second, the whole genome was successfully amplified with Nt·BstNBI (6 U), betaine (1 M) and trehalose (60 mM) for the first time. Third, we achieved 10 pg sensitivity for the first time after adding a small molecular beacon that spontaneously undergoes a conformational change when hybridizing to target, and the practical test validated the assay's application. The small molecular beacon has a similar melting temperature to the reaction temperature, but is approximately 10 bp shorter than the length of a traditional molecular beacon. A new threshold regulation was also established for isothermal conditions. Finally, we established a thermodynamic model for designing small molecular beacons. This multistate model is more correct than the traditional algorithm. This theoretical and practical basis will help us to monitor SMB-NEMA in a quantitative way. In summary, our SMB-NEMA method allows the simple, specific and sensitive assessment of isothermal DNA quantification.

5.
Anal Biochem ; 443(2): 243-8, 2013 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-24050969

RESUMO

In this study, a novel single universal primer multiplex ligation-dependent probe amplification (SUP-MLPA) technique that uses only one universal primer to perform multiplex polymerase chain reaction (PCR) was developed. Two reversely complementary common sequences were designed on the 5' or 3' end of the ligation probes (LPs), which allowed the ligation products to be amplified through only a single universal primer (SUP). SUP-MLPA products were analyzed on sequencing gel electrophoresis with extraordinary resolution. This method avoided the high expenses associated with capillary electrophoresis, which was the commonly used detection instrument. In comparison with conventional multiplex PCR, which suffers from low sensitivity, nonspecificity, and amplification disparity, SUP-MLPA had higher specificity and sensitivity and a low detection limit of 0.1 ng for detecting single crop species when screening the presence of genetically modified crops. We also studied the effect of different lengths of stuffer sequences on the probes for the first time. Through comparing the results of quantitative PCR, the LPs with different stuffer sequences did not affect the ligation efficiency, which further increased the multiplicity of this assay. The improved SUP-MLPA and sequencing gel electrophoresis method will be useful for food and animal feed identification, bacterial detection, and verification of genetic modification status of crops.


Assuntos
Primers do DNA/genética , Eletroforese em Gel de Poliacrilamida/métodos , Reação em Cadeia da Polimerase Multiplex/métodos , Plantas Geneticamente Modificadas/genética , Soja/genética , Zea mays/genética , Sequência de Bases , Produtos Agrícolas/genética , DNA de Plantas/genética , DNA de Plantas/isolamento & purificação , Dados de Sequência Molecular
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