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1.
ACS Appl Mater Interfaces ; 10(11): 9435-9443, 2018 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-29528216

RESUMO

Lithium-sulfur (Li-S) battery is regarded as one of the most promising next-generation efficient energy storage systems because of its ultrahigh theoretical capacity of 1675 mAh/g and energy density of 2600 Wh/kg accompanied by the environmental benignity and abundance from natural sulfur. However, the insulating nature of sulfur and the dissolution of the polysulfides Li2S n (4 ≤ n ≤ 8) seriously restrict its practical application. The metastable small sulfur molecules (S2-4) stored in microporous carbon (pore size of <0.6 nm) as the active materials can avoid the production of the soluble polysulfide and solve the shuttle effect thoroughly. In addition, the conductivity of sulfur can be also improved. However, the preparation of microporous carbon materials with reasonable pore size and unique morphology for efficiently encapsulating S2-4 is still challenging. Herein, three flowerlike microporous nitrogen-doped carbon nanosheets with the pore size of <0.6 nm (namely, FMNCN-800, -900, and -1000) as the cathode materials in Li-S batteries were obtained from temperature-dependent carbonization of the metal-organic framework (MOF), Zn-TDPAT, which was from the simply reflux reaction of N-rich ligand H6TDPAT with Zn(II) salt. Our study showed that the FMNCN-900 from carbonization of Zn-TDPAT at 900 °C has suitable pore volume and nitrogen content, accommodating small S2-4 molecules in its micropores with the mass uptake of about 45%. Meanwhile, the appropriate amount of the nitrogen doping and the unique nanostructure of the flowerlike carbon nanosheet in the FMNCN-900 can effectively support its fast electronic transmission and lithium-ion conduction. The resulting S@FMNCN-900 composite cathode material presents the excellent electrochemical property in the Li-S battery (here the carbonate as electrolytes) with a reversible capacity of about 1220 mAh/g at 0.1C after 200 cycles and even 727 mAh/g at 2C after the long-term cycle of 1000 with only around 0.02% capacity loss per cycle. Obviously, the results indicate that the delicate construction of MOF-derived nitrogen-doped microporous carbon nanosheet is a promising strategy to develop novel electrode material for high-performing Li-S batteries.

2.
ACS Appl Mater Interfaces ; 9(34): 29374-29379, 2017 Aug 30.
Artigo em Inglês | MEDLINE | ID: mdl-28792198

RESUMO

The removal of acetylene from the industrial feed gas to purify the ethylene is an important and challenging issue. The adsorption-based separation is a more environmentally friendly and cost-effective method compared to the current removal approaches such as partial hydrogenation and solvent extraction, while facing the challenge of developing materials with high C2H2/C2H4 selectivity and C2H2 capacity. Herein, by expanding mixed-metal organic frameworks (M'MOFs) structure with high C2H2/C2H4 selectivity, we report a pillar-layered MOF, {[Cd5(MPCZ)2(BDC)3(NO3)2(H2O)4]·G}n (MECS-5), which not only inherits the sieving effects of M'MOF series but also develops its own characteristic-the 2D layer with expanding space and the plane pore-partition group to "cover" it. MECS-5 shows higher ideal adsorption solution theory C2H2/C2H4 selectivity than the most reported MOFs, especially more than 5 times higher than MOF-74 series while displaying great enhancement in the C2H2 capacity, more than 2 times higher compared to the M'MOF. The column breakthrough experiment further proves the possibility of MECS-5a for real industrial ethylene purification.

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