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1.
Artículo en Inglés | MEDLINE | ID: mdl-39028897

RESUMEN

We successfully synthesized hybrid MXene-K-CNT composites composed of alkalized two-dimensional (2D) metal carbide and carbon nanotubes (CNTs), which were employed as host materials for lithium-sulfur (Li-S) battery cathodes. The unique three-dimensional (3D) intercalated structure through electrostatic interactions by K+ ions in conjunction with the scaffolding effect provided by CNTs effectively inhibited the self-stacking of MXene nanosheets, resulting in an enhanced specific surface area (SSA) and ion transport capability. Moreover, the addition of CNTs and in situ-grown TiO2 considerably improved the conductivity of the cathode material. K+ ion etching created a more hierarchical porous structure in MXene, which further enhanced the SSA. The 3D framework effectively confined S embedded between nanosheet layers and suppressed volume changes of the cathode composite during charging/discharging processes. This combination of CNTs and alkalized nanosheets functioned as a physical and chemical dual adsorption system for lithium polysulfides (LiPSs). When subjected to a high current at 1.0C, S@MXene-K-0.5CNT with S-loaded of 1.2 mg cm-2 had an initial capacity of 919.6 mAh g-1 and capacity decay rate of merely 0.052% per cycle after 1000 cycles. Moreover, S@MXene-K-0.5CNT maintained good cycling stability even at a high current of up to 5.0C. These impressive results highlight the potential of alkalized 2D MXene nanosheets intercalated with CNTs as highly promising cathode materials for Li-S batteries. The study findings also have prospects for the development of next-generation Li-S batteries with high energy density and prolonged lifespans.

2.
ACS Appl Mater Interfaces ; 14(37): 42102-42112, 2022 Sep 21.
Artículo en Inglés | MEDLINE | ID: mdl-36097412

RESUMEN

AlH3 is a metastable hydride with a theoretical hydrogen capacity of 10.01 wt % and is very easy to decompose during ball milling especially in the presence of many catalysts, which will lead to the attenuation of the available hydrogen capacity. In this work, AlH3 was ball milled in air (called "air-milling") with layered Ti3C2 to prepare a Ti3C2-catalyzed AlH3 hydrogen storage material. Such air-milled and Ti3C2-catalyzed AlH3 possesses excellent hydrogen storage performances, with a low initial decomposition temperature of just 61 °C and a high hydrogen release capacity of 8.1 wt %. In addition, 6.9 wt % of hydrogen can be released within 20 min at constantly 100 °C, with a low activation energy as low as 40 kJ mol-1. Air-milling will lead to the formation of an Al2O3 oxide layer on the AlH3 particles, which will prevent continuous decomposition of AlH3 when milling with active layered Ti3C2. The layered Ti3C2 will grip on and intrude into the AlH3 particle oxide layers and then catalyze the decomposition of AlH3 during heating. The strategy employing air-milling as a synthesis method and utilizing layered Ti3C2 as a catalyst in this work can solve the key issue of severe decomposition during ball milling with catalysts economically and conveniently and thus achieve both high-capacity and low-temperature hydrogen storage of AlH3. This air-milling method is also effective for other active catalysts toward both reducing the decomposition temperature and increasing the available hydrogen capacity of AlH3.

3.
Nanomaterials (Basel) ; 12(15)2022 Aug 05.
Artículo en Inglés | MEDLINE | ID: mdl-35957132

RESUMEN

The development of novel catalysts for degrading organic contaminants in water is a current hot topic in photocatalysis research for environmental protection. In this study, C3N5 nanosheet/Ag2CO3 nanocomposites (CNAC-X) were used as efficient photocatalysts for the visible-light-driven degradation of methylene blue (MB), and tetracycline hydrochloride (TC-HCl) was synthesized for the first time using a simple thermal oxidative exfoliation and in situ deposition method. Due to the synergistic effect of nanosheet structures, carbon defects, and Z-scheme heterojunctions, CNAC-10 exhibited the highest photocatalytic activity, with photodegradation efficiencies of 96.5% and 97.6% for MB (60 mg/L) and TC-HCl (50 mg/L) within 90 and 100 min, respectively. The radical trapping experiments showed that ·O2- and h+ played major roles in the photocatalytic effect of the CNAC-10 system. Furthermore, intermediates in the photodegradation of MB and TC-HCl were investigated to determine possible mineralization pathways. The results indicated that C3N5 nanosheet/Ag2CO3 photocatalysts prepared in this work could provide an effective reference for the treatment of organic wastewater.

4.
Nanomaterials (Basel) ; 12(8)2022 Apr 12.
Artículo en Inglés | MEDLINE | ID: mdl-35458031

RESUMEN

Compared with the polycrystalline system, the single-crystalline ternary cathode material has better cycle stability because the only primary particles without grain boundaries effectively alleviate the formation of micro/nanocracks and retain better structural integrity. Therefore, it has received extensive research attention. There is no consistent result whether tungsten oxide acts as doping and/or coating from the surface modification of the polycrystalline system. Meanwhile, there is no report on the surface modification of the single-crystalline system by tungsten oxide. In this paper, multirole surface modification of single-crystalline nickel-rich ternary cathode material LiNi0.6Co0.2Mn0.2O2 by WO3 is studied by a simple method of adding WO3 followed by calcination. The results show that with the change in the amount of WO3 added, single-crystalline nickel-rich ternary cathode material can be separately doped, separately coated, and both doped and coated. Either doping or coating effectively enhances the structural stability, reduces the polarization of the material, and improves the lithium-ion diffusion kinetics, thus improving the cycle stability and rate performance of the battery. Interestingly, both doping and coating (for SC-NCM622-0.5%WO3) do not show a more excellent synergistic effect, while the single coating (for SC-NCM622-1.0%WO3) after eliminating the rock-salt phase layer performs the most excellent modification effect.

5.
Bull Environ Contam Toxicol ; 109(1): 142-148, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35305129

RESUMEN

Bauxite residue is generated from alumina production in the alumina refining industry by the Bayer process, which requires a large amount of land resource and causes serious environmental problems. In this paper, a novel recycling strategy is proposed to rehabilitate the land and produce the polyaluminium ferric sulfate (PAFS) and siliceous gypsum byproducts from the bauxite residue. The batch experiments reveal that the maximum Cr(VI) removal efficiency of as-prepared PAFS can reach 95.80% with an initial concentration of 10.41 mg/L. In addition, the non-toxic siliceous gypsum should be an ideal raw material for cement plants. Various characterizations (e.g., SEM, FTIR, and XRD) are employed to reveal the mechanism of synthesis PAFS and their Cr(VI) removal performance. Consequently, this paper provides a deep insight into the utilization of bauxite residue as a resource and gives a new strategy for preparing PAFS and gypsum from bauxite residue.


Asunto(s)
Óxido de Aluminio , Aguas Residuales , Sulfato de Calcio , Cromo , Compuestos Férricos
6.
Front Chem ; 9: 775537, 2021.
Artículo en Inglés | MEDLINE | ID: mdl-34722466

RESUMEN

Mg-Li alloy possesses a high hydrogen capacity. However, the hydrogenation and dehydrogenation performances are still far from practical application. In this work, Mg2Si (MS) and graphene (G) were employed together to synergistically improve the hydrogen storage properties of Mg-Li alloy. The structures of the samples were studied by XRD and SEM methods. The hydrogen storage performances of the samples were studied by nonisothermal and isothermal hydrogenation and dehydrogenation, thermal analysis, respectively. It is shown that the onset dehydrogenation temperature of Mg-Li alloy was synergistically reduced from 360°C to 310°C after co-addition of Mg2Si and graphene. At a constant temperature of 325°C, the Mg-Li-MS-G composite can release 2.7 wt.% of hydrogen within 2 h, while only 0.2 wt.% of hydrogen is released for the undoped Mg-Li alloy. The hydrogenation activation energy of the Mg-Li-MS-G composite was calculated to be 86.5 kJ mol-1. Microstructure and hydrogen storage properties studies show that graphene can act as a grinding aid during the ball milling process, which leads to a smaller particle size for the composites. This work demonstrates that coaddition of Mg2Si and graphene can synergistically improve the hydrogen storage properties of Mg-Si alloy and offers an insight into the role of graphene in the Mg-Li-MS-G composite.

7.
ACS Appl Mater Interfaces ; 13(10): 11901-11910, 2021 Mar 17.
Artículo en Inglés | MEDLINE | ID: mdl-33660995

RESUMEN

The Mg17Al12-BaO composite is synthesized via mechanical milling and the effect of BaO on the hydrogen sorption properties of Mg17Al12 is studied. Experimentally, we prepare the Mg17Al12-Ba, Mg17Al12-BaO, Mg17Al12-BaF2, and Mg17Al12-BaCl2 mixtures and find that the Mg17Al12-BaO composite shows a superior hydrogen storage performance. For instance, the hydrogenation (dehydrogenation) enthalpy of the Mg17Al12 decreases from 62.4 (91.2) to 58.6 (71.7) kJ mol-1 after adding BaO. When 1.0 wt % of H2 is absorbed/desorbed, the hydrogen absorption/desorption temperature of the Mg17Al12-BaO is 181/271 °C, which is 73/37 °C lower than that of the Mg17Al12. Furthermore, the catalytic mechanism of BaO on the hydrogenation of Mg17Al12 (110) surface is investigated by density functional theory (DFT). Calculations indicate that compared with the Mg17Al12 (110) surface, the adsorption energy and dissociation barrier of hydrogen on the Mg17Al12-BaO (110) surface are both improved significantly. Our experimental and theoretical results are helpful for understanding the effect of metal oxide on hydrogen storage properties of Mg17Al12.

8.
ACS Appl Mater Interfaces ; 13(11): 13235-13247, 2021 Mar 24.
Artículo en Inglés | MEDLINE | ID: mdl-33720702

RESUMEN

Two-dimensional vanadium carbide (V2C) and titanium carbide (Ti3C2) MXenes were first synthesized by exfoliating V2AlC or Ti3AlC2 and then introduced jointly into magnesium hydride (MgH2) to tailor the hydrogen desorption/absorption performances of MgH2. The as-prepared MgH2-V2C-Ti3C2 composites show much better hydrogen storage performances than pure MgH2. MgH2 with addition of 10 wt % of 2V2C/Ti3C2 initiates hydrogen desorption at around 180 °C; 5.1 wt % of hydrogen was desorbed within 60 min at 225 °C, while 5.8 wt % was desorbed within 2 min at 300 °C. Under 6 MPa H2, the dehydrided MgH2-2V2C/Ti3C2 can start to recover hydrogen at room temperature, and 5.1 wt % of H2 is obtained within 20 s at a constant temperature of 40 °C. The reversible capacity (6.3 wt %) does not decline for up to 10 cycles, which shows excellent cycling stability. The addition of 2V2C/Ti3C2 can remarkably lower the activation energy for the hydrogen desorption reaction of MgH2 by 37% and slightly reduce the hydrogen desorption reaction enthalpy by 2 kJ mol-1 H2. It was demonstrated that the combination of V2C and Ti3C2 promotes the hydrogen-releasing process of MgH2 compared with addition of only V2C or Ti3C2, while Ti3C2 impacts MgH2 more significantly than V2C in the hydrogen absorption process of MgH2 at ambient temperatures. A possible mechanism in the hydrogen release and uptake of the MgH2-V2C-Ti3C2 system was proposed as follows: hydrogen atoms or molecules may preferentially transfer through the MgH2/V2C/Ti3C2 triple-grain boundaries during the desorption process and through the Mg/Ti3C2 interfaces during the absorption process. Microstructure studies indicated that V2C and Ti3C2 mainly act as efficient catalysts for MgH2. This work provides an insight into the hydrogen storage behaviors and mechanisms of MgH2 boosted by a combination of two MXenes.

9.
Front Chem ; 8: 207, 2020.
Artículo en Inglés | MEDLINE | ID: mdl-32266219

RESUMEN

To improve the hydrogen storage properties of Mg/MgH2, a Ni and TiO2 co-doped reduced graphene oxide [(Ni-TiO2)@rGO] nanocomposite is synthesized by a facile impregnation method and introduced into Mg via ball milling. The results demonstrated that the dispersive distribution of Ni and TiO2 with a particle size of 20-200 nm in the reduced graphene oxide matrix led to superior catalytic effects on the hydrogen storage properties of Mg-(Ni-TiO2)@rGO. The initial hydrogenation/dehydrogenation temperature for Mg-(Ni-TiO2)@rGO decreased to 323/479 K, 75/84 K lower than that of the additive-free sample. The hydrogen desorption capacity of the Mg-(Ni-TiO2)@rGO composite released 1.47 wt.% within 120 min at 498 K. When the temperature was increased to 523 K, the hydrogen desorption capacity increased to 4.30 wt.% within 30 min. A hydrogenation/dehydrogenation apparent activation energy of 47.0/99.3 kJ·mol-1 was obtained for the Mg-(Ni-TiO2)@rGO composite. The improvement in hydrogenation and dehydrogenation for the Mg-(Ni-TiO2)@rGO composite was due to the reduction of the apparent activation energy by the catalytic action of (Ni-TiO2)@rGO.

10.
Front Chem ; 7: 892, 2019.
Artículo en Inglés | MEDLINE | ID: mdl-32010663

RESUMEN

Aluminum hydride (AlH3) is a promising candidate for hydrogen storage due to its high hydrogen density of 10 wt%. Several polymorphs of AlH3 (e.g., α, ß, and γ) have been successfully synthesized by wet chemical reaction of LiAlH4 and AlCl3 in ether solution followed by desolvation. However, the synthesis process of α'-AlH3 from wet chemicals still remains unclear. In the present work, α'-AlH3 was synthesized first by the formation of the etherate AlH3 through a reaction of LiAlH4 and AlCl3 in ether solution. Then, the etherate AlH3 was heated at 60°C under an ether gas atmosphere and in the presence of excess LiAlH4 to remove the ether ligand. Finally, α'-AlH3 was obtained by ether washing to remove the excess LiAlH4. It is suggested that the desolvation of the etherate AlH3 under an ether gas atmosphere is essential for the formation of α'-AlH3 from the etherate AlH3. The as-synthesized α'-AlH3 takes the form of rod-like particles and can release 7.7 wt% hydrogen in the temperature range 120-200°C.

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