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1.
Chem Sci ; 15(3): 1123-1131, 2024 Jan 17.
Article in English | MEDLINE | ID: mdl-38239697

ABSTRACT

Exploring economical, efficient, and stable electrocatalysts for the seawater hydrogen evolution reaction (HER) is highly desirable but is challenging. In this study, a Mo cation doped Ni0.85Se/MoSe2 heterostructural electrocatalyst, Mox-Ni0.85Se/MoSe2, was successfully prepared by simultaneously doping Mo cations into the Ni0.85Se lattice (Mox-Ni0.85Se) and growing atomic MoSe2 nanosheets epitaxially at the edge of the Mox-Ni0.85Se. Such an Mox-Ni0.85Se/MoSe2 catalyst requires only 110 mV to drive current densities of 10 mA cm-2 in alkaline simulated seawater, and shows almost no obvious degradation after 80 h at 20 mA cm-2. The experimental results, combined with the density functional theory calculations, reveal that the Mox-Ni0.85Se/MoSe2 heterostructure will generate an interfacial electric field to facilitate the electron transfer, thus reducing the water dissociation barrier. Significantly, the heteroatomic Mo-doping in the Ni0.85Se can regulate the local electronic configuration of the Mox-Ni0.85Se/MoSe2 heterostructure catalyst by altering the coordination environment and orbital hybridization, thereby weakening the bonding interaction between the Cl and Se/Mo. This synergistic effect for the Mox-Ni0.85Se/MoSe2 heterostructure will simultaneously enhance the catalytic activity and durability, without poisoning or corrosion of the chloride ions.

2.
Nat Commun ; 9(1): 4082, 2018 10 04.
Article in English | MEDLINE | ID: mdl-30287817

ABSTRACT

The low-cost room-temperature sodium-sulfur battery system is arousing extensive interest owing to its promise for large-scale applications. Although significant efforts have been made, resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging. Here, a sulfur host comprised of atomic cobalt-decorated hollow carbon nanospheres is synthesized to enhance sulfur reactivity and to electrocatalytically reduce polysulfide into the final product, sodium sulfide. The constructed sulfur cathode delivers an initial reversible capacity of 1081 mA h g-1 with 64.7% sulfur utilization rate; significantly, the cell retained a high reversible capacity of 508 mA h g-1 at 100 mA g-1 after 600 cycles. An excellent rate capability is achieved with an average capacity of 220.3 mA h g-1 at the high current density of 5 A g-1. Moreover, the electrocatalytic effects of atomic cobalt are clearly evidenced by operando Raman spectroscopy, synchrotron X-ray diffraction, and density functional theory.

3.
ACS Appl Mater Interfaces ; 9(29): 24446-24450, 2017 Jul 26.
Article in English | MEDLINE | ID: mdl-28699731

ABSTRACT

Room-temperature sodium-sulfur batteries are competitive candidates for large-scale stationary energy storage because of their low price and high theoretical capacity. Herein, pure S nanosheet cathodes can be grown in situ on three-dimensional Cu foam substrate with the condensation between binary polymeric binders, serving as a model system to investigate the formation and electrochemical mechanism of unique S nanosheets on the Cu current collectors. On the basis of the confirmed conversion reactions to Na2S, The constructed cathode exhibits ultrahigh initial discharge/charge capacity of 3189/1403 mAh g-1. These results suggest that there is great potential to optimize S cathode by exploiting low-cost Cu substrates instead of conventional Al current collectors.

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