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High-Performance Aqueous Zinc-Manganese Battery with Reversible Mn²⁺/Mn⁴⁺ Double Redox Achieved by Carbon Coated MnO_x Nanoparticles.

ABSTRACT: There is an urgent need for low-cost, high-energy-density, environmentally friendly energy storage devices to fulfill the rapidly increasing need for electrical energy storage. Multi-electron redox is considerably crucial for the development of high-energy-density cathodes. Here we present high-performance aqueous zinc-manganese batteries with reversible Mn²⁺/Mn⁴⁺ double redox. The active Mn⁴⁺ is generated in situ from the Mn²⁺-containing MnO_x nanoparticles and electrolyte. Benefitting from the low crystallinity of the birnessite-type MnO₂ as well as the electrolyte with Mn²⁺ additive, the MnO_x cathode achieves an ultrahigh energy density with a peak of 845.1 Wh kg^-1 and an ultralong lifespan of 1500 cycles. The combination of electrochemical measurements and material characterization reveals the reversible Mn²⁺/Mn⁴⁺ double redox (birnessite-type MnO₂↔ monoclinic MnOOH and spinel ZnMn₂O₄ ↔ Mn²⁺ ions). The reversible Mn²⁺/Mn⁴⁺ double redox electrode reaction mechanism offers new opportunities for the design of low-cost, high-energy-density cathodes for advanced rechargeable aqueous batteries.

SUBMITTER: Huang J

PROVIDER: S-EPMC7770770 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Transition metal oxides are characterized by an acute structure and composition dependent electrocatalytic activity toward the oxygen evolution (OER) and oxygen reduction (ORR) reactions. For instance, Mn containing oxides are among the most active ORR catalysts, while Ni based compounds tend to show high activity toward the OER in alkaline solutions. In this study, we show that incorporation of Ni into α-MnO2, by adding Ni precursor into the Mn-containing hydrothermal solution, can generate distinctive sites with different electronic configurations and contrasting electrocatalytic activity. The structure and composition of the Ni modified hollandite α-MnO2 phase were investigated by X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), transmission electron microscopy coupled to energy-dispersive X-ray spectroscopy (TEM-EDX), inductively coupled plasma-optical emission spectroscopy (ICP-OES), and X-ray photoelectron spectroscopy (XPS). Our analysis suggests that Mn replacement by Ni into the α-MnO2 lattice (site A) occurs up to approximately 5% of the total Mn content, while further increasing Ni content promotes the nucleation of separate Ni phases (site B). XAS and XRD show that the introduction of sites A and B have a negligible effect on the overall Mn oxidation state and bonding characteristics, while very subtle changes in the XPS spectra appear to suggest changes in the electronic configuration upon Ni incorporation into the α-MnO2 lattice. On the other hand, changes in the electronic structure promoted by site A have a significant impact in the pseudocapacitive responses obtained by cyclic voltammetry in KOH solution at pH 13, revealing the appearance of Mn 3d orbitals at the energy (potential) range relevant to the ORR. The evolution of Mn 3d upon Ni replacement significantly increases the catalytic activity of α-MnO2 toward the ORR. Interestingly, the formation of segregated Ni phases (site B) leads to a decrease in the ORR activity while increasing the OER rate.

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High-Performance Aqueous Zinc-Manganese Battery with Reversible Mn²⁺/Mn⁴⁺ Double Redox Achieved by Carbon Coated MnO_x Nanoparticles.

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High-Performance Aqueous Zinc-Manganese Battery with Reversible Mn2+/Mn4+ Double Redox Achieved by Carbon Coated MnOx Nanoparticles.

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High-Performance Aqueous Zinc-Manganese Battery with Reversible Mn²⁺/Mn⁴⁺ Double Redox Achieved by Carbon Coated MnO_x Nanoparticles.