Microwave-Assisted Doping Engineering Construction of Spinel-Structured Nonstoichiometric Manganese Cobaltite with Mixed 1D/2D Morphology for Supercapacitor Application

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Abstract
High-performance electrode materials are fundamental to improving supercapacitor performance, serving as key factors in developing devices with high energy density, high power density, and excellent cyclic stability. Non-stoichiometric spinels with phase deficiencies can achieve electrochemical performance that surpasses that of stoichiometric materials, owing to their unique structural characteristics. In this study, we used a microwave-assisted method to synthesize a high-performance non-stoichiometric spinel material with phase deficiencies, Mn0.5Co2.5O4, which displayed a wide potential window (1.13 V in a traditional aqueous three-electrode system) and high specific capacitance (716.9 F g−1 at 1 A g−1). More critically, through microwave-assisted doping engineering, nickel was successfully doped into the phase-deficient Mn0.5Co2.5O4, resulting in a spinel material, Ni−Mn0.5Co2.5O4, with significant lattice defects and a mixed 1D/2D morphology. The doping of nickel effectively promoted the high-state conversion of manganese valence states within the manganese cobaltite material, substantially increasing the quantity of highly active Co3+ ions. These changes led to an increase in the density of reactive sites, effectively promoting synergistic interactions, thereby significantly enhancing the material’s conductivity and energy storage performance. The specific capacitance of Ni−Mn0.5Co2.5O4 reached 1180.6 F g−1 at 1 A g−1, a 64.7% improvement over the original Mn0.5Co2.5O4; at a high current density of 10 A g−1, the capacitance increased by 14.3%. Notably, the charge transfer resistance was reduced by a factor of 41.6. After 5000 cycles of testing, the capacity retention stood at 79.2%. This work reveals the effectiveness of microwave-assisted doping engineering in constructing high-performance non-stoichiometric spinel-type bimetallic oxide materials, offering advanced strategies for the development of high-performance electrode materials.
Funding Information
  • Natural Science Foundation of Guangdong Province (2022A1515011562, Yuerong Office Letter [2020] 161, 060302132314, 060302132103, 2024KQNCX135, 2024B01043, GDNRC [2023] 51)
  • Guangdong Provincial Special Fund for promoting high-quality economic development (2022A1515011562, Yuerong Office Letter [2020] 161, 060302132314, 060302132103, 2024KQNCX135, 2024B01043, GDNRC [2023] 51)
  • Scientific Research Start-up Foundation of Guangdong Ocean University (2022A1515011562, Yuerong Office Letter [2020] 161, 060302132314, 060302132103, 2024KQNCX135, 2024B01043, GDNRC [2023] 51)
  • Guangdong University Young Innovative Talents Program Project 2024 (2022A1515011562, Yuerong Office Letter [2020] 161, 060302132314, 060302132103, 2024KQNCX135, 2024B01043, GDNRC [2023] 51)
  • Zhanjiang Non-funded Science and Technology Research Project (2022A1515011562, Yuerong Office Letter [2020] 161, 060302132314, 060302132103, 2024KQNCX135, 2024B01043, GDNRC [2023] 51)
  • Special Funds for Marine Economic Development of Guangdong Province (2022A1515011562, Yuerong Office Letter [2020] 161, 060302132314, 060302132103, 2024KQNCX135, 2024B01043, GDNRC [2023] 51)

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