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1.
J Colloid Interface Sci ; 663: 566-576, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38428114

RESUMO

Transition metal spinel oxides were engineered with active elements as bifunctional water splitting electrocatalysts to deliver superior intrinsic activity, stability, and improved conductivity to support green hydrogen production. In this study, we reported the ternary metal Ni-Fe-Co spinel oxide electrocatalysts prepared by defect engineering strategy with rich and deficient Na+ ions, termed NFCO-Na and NFCO, which suggest the formation of defects with Na+ forming tensile strain. The Na-rich NiFeCoO4 spinel oxide reveals lattice expansion, resulting in the formation of a defective crystal structure, suggesting higher electrocatalytic active sites. The spherical NFCO-Na electrocatalysts exhibit lower OER and HER overpotentials of 248 mV and 153 mV at 10 mA cm-2 and smaller Tafel slope values of about 78 mV dec-1 and 129 mV dec-1, respectively. Notably, the bifunctional NFCO-Na electrocatalyst requires a minimum cell voltage of about 1.67 V to drive a current density of 10 mA cm-2. The present work highlights the significant electrochemical activity of defect-engineered ternary metal oxides, which can be further upgraded as highly active electrocatalysts for water splitting applications.

2.
Chemosphere ; 352: 141233, 2024 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-38266882

RESUMO

Hydrogen production from water splitting combined with renewable electricity can provide a viable solution to the energy crisis. A novel MoS2/NiS2/Ni3S4 heterostructure is designed as a bifunctional electrocatalyst by facile hydrothermal method to demonstrate excellent electrocatalytic performance towards overall water splitting applications. MoS2/NiS2/Ni3S4 heterostructure necessitates a low overpotential of 81 mV and 210 mV to attain a current density of 10 mA cm-2 during the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively. Consequently, the MoS2/NiS2/Ni3S4 heterostructure-based electrolyzer shows a low cell voltage of 1.54 V at 10 mA cm-2. The present work highlights the significance of the heterostructure configuration of transition metal sulfide-based electrocatalysts for electrochemical overall water splitting applications.


Assuntos
Eletricidade , Molibdênio , Hidrogênio , Oxigênio , Sulfetos
3.
Front Chem ; 11: 1122150, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36874069

RESUMO

Hydrogen has become an indispensable aspect of sustainable energy resources due to depleting fossil fuels and increasing pollution. Since hydrogen storage and transport is a major hindrance to expanding its applicability, green ammonia produced by electrochemical method is sourced as an efficient hydrogen carrier. Several heterostructured electrocatalysts are designed to achieve significantly higher electrocatalytic nitrogen reduction (NRR) activity for electrochemical ammonia production. In this study, we controlled the nitrogen reduction performances of Mo2C-Mo2N heterostructure electrocatalyst prepared by a simple one pot synthesis method. The prepared Mo2C-Mo2N0.92 heterostructure nanocomposites show clear phase formation for Mo2C and Mo2N0.92, respectively. The prepared Mo2C-Mo2N0.92 electrocatalysts deliver a maximum ammonia yield of about 9.6 µg h-1 cm-2 and a Faradaic efficiency (FE) of about 10.15%. The study reveals the improved nitrogen reduction performances of Mo2C-Mo2N0.92 electrocatalysts due to the combined activity of the Mo2C and Mo2N0.92 phases. In addition, the ammonia production from Mo2C-Mo2N0.92 electrocatalysts is intended by the associative nitrogen reduction mechanism on Mo2C phase and by Mars-van-Krevelen mechanism on Mo2N0.92 phase, respectively. This study suggests the importance of precisely tuning the electrocatalyst by heterostructure strategy to substantially achieve higher nitrogen reduction electrocatalytic activity.

4.
ACS Appl Mater Interfaces ; 14(28): 31889-31899, 2022 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-35816758

RESUMO

Ammonia is a suitable hydrogen carrier with each molecule accounting for up to 17.65% of hydrogen by mass. Among various potential ammonia production methods, we adopt the photoelectrochemical (PEC) technique, which uses solar energy as well as electricity to efficiently synthesize ammonia under ambient conditions. In this article, we report MoS2@La2Zr2O7 heterostructures designed by incorporating two-dimensional (2D)-MoS2 nanoflakes on La2Zr2O7 nanofibers (MoS2@LZO) as photoelectrocatalysts. The MoS2@LZO heterostructures are synthesized by a facile hydrothermal route with electrospun La2Zr2O7 nanofibers and Mo precursors. The MoS2@LZO heterostructures work synergistically to amend the drawbacks of the individual MoS2 electrocatalysts. In addition, the harmonious activity of the mixed phase of pyrochlore/defect fluorite-structured La2Zr2O7 nanofibers generates an interface that aids in increased electrocatalytic activity by enriching oxygen vacancies in the system. The MoS2@LZO electrocatalyst exhibits an enhanced Faradaic efficiency and ammonia yield of approximately 2.25% and 10.4 µg h-1 cm-2, respectively, compared to their corresponding pristine samples. Therefore, the mechanism of improving the PEC ammonia production performance by coupling oxygen-vacant sites to the 2D-semiconductor-based electrocatalysts has been achieved. This work provides a facile strategy to improve the activity of PEC catalysts by designing an efficient heterostructure interface for PEC applications.

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