Phosphorus-Induced One-Step Synthesis of NiCo2S4 Electrode Material for Efficient Hydrazine-Assisted Hydrogen Production
Rational control of the reaction parameters is highly important for synthesizing active electrocatalysts. NiCo2S4 is an excellent spinel-based electrocatalyst that is usually prepared through a two-step synthesis. Herein, a one-step hydrothermal route is reported to synthesize P-incorporated NiCo2S4...
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Veröffentlicht in: | Inorganic chemistry 2023-10, Vol.62 (39), p.16149-16160 |
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Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | Rational control of the reaction parameters is highly important for synthesizing active electrocatalysts. NiCo2S4 is an excellent spinel-based electrocatalyst that is usually prepared through a two-step synthesis. Herein, a one-step hydrothermal route is reported to synthesize P-incorporated NiCo2S4. We discovered that the inclusion of P caused formation of the NiCo2S4 phase in a single step. Computational studies were performed to comprehend the mechanism of phase formation and to examine the energetics of lattice formation. Upon incorporation of the optimum amount of P, the stability of the NiCo2S4 lattice was found to increase steadily. In addition, the Bader charges on both the metal atoms Co and Ni in NiCo2S4 and P-incorporated NiCo2S4 were compared. The results show that replacing S with the optimal amount of P leads to a reduction in charge on both metal atoms, which can contribute to a more stable lattice formation. Further, the electrochemical performance of the as-synthesized materials was evaluated. Among the as-synthesized nickel cobalt sulfides, P-incorporated NiCo2S4 exhibits excellent activity toward hydrazine oxidation with an onset potential of 0.15 V vs RHE without the assistance of electrochemically active substrates like Ni or Co foam. In addition to the facile synthesis method, P-incorporated NiCo2S4 requires a very low cell voltage of 0.24 V to attain a current density of 10 mA cm–2 for hydrazine-assisted hydrogen production in a two-electrode cell. The free energy profile of the stepwise HzOR has been investigated in detail. The computational results suggested that HzOR on P-incorporated NiCo2S4 was more feasible than HzOR on NiCo2S4, and these findings corroborate the experimental evidence. |
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ISSN: | 0020-1669 1520-510X |
DOI: | 10.1021/acs.inorgchem.3c02418 |