Zn Metal Atom Doping on the Surface Plane of One-Dimesional NiMoO₄ Nanorods with Improved Redox Chemistry
2020
Sharma, Pratigya | Minakshi Sundaram, Manickam | Watcharatharapong, Teeraphat | Laird, Damian | Euchner, Holger | Ahuja, Rajeev
The effect of zinc (Zn) doping and defect formation on the surface of nickel molybdate (NiMoO₄) structures with varying Zn content has been studied to produce one-dimensional electrodes and catalysts for electrochemical energy storage and ethanol oxidation, respectively. Zn-doped nickel molybdate (Ni₁₋ₓZnₓMoO₄, where x = 0.1, 0.2, 0.4, and 0.6) nanorods were synthesized by a simple wet chemical route. The optimal amount of Zn is found to be around 0.25 above which the NiMoO₄ becomes unstable, resulting in poor electrochemical activity. This result agrees with our density functional theory calculations in which the thermodynamic stability reveals that Ni₁₋ₓZnₓMoO₄ crystallized in the β-NiMoO₄ phase and is found to be stable for x≤0.25. Analytical techniques show direct evidence of the presence of Zn in the NiMoO₄ nanorods, which subtly alter the electrocatalytic activity. Compared with pristine NiMoO₄, Zn-doped NiMoO₄ with the optimized Zn content was tested as an electrode for an asymmetric supercapacitor and demonstrated an enhanced specific capacitance of 122 F g–¹ with a high specific energy density of 43 W h kg–¹ at a high power density of 384 W kg–¹. Our calculations suggest that the good conductivity from Zn doping is attributed to the formation of excess oxygen vacancies and dopants play an important role in enhancing the charge transfer between the surface and OH– ions from the electrolyte. We report electrochemical testing, material characterization, and computational insights and demonstrate that the appropriate amount of Zn in NiMoO₄ can improve the storage capacity (∼15%) due to oxygen vacancy interactions.
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