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Inhibition of oxygen dimerization by local symmetry tuning in Li-rich layered oxides for improved stability.

ABSTRACT: Li-rich layered oxide cathode materials show high capacities in lithium-ion batteries owing to the contribution of the oxygen redox reaction. However, structural accommodation of this reaction usually results in O-O dimerization, leading to oxygen release and poor electrochemical performance. In this study, we propose a new structural response mechanism inhibiting O-O dimerization for the oxygen redox reaction by tuning the local symmetry around the oxygen ions. Compared with regular Li₂RuO₃, the structural response of the as-prepared local-symmetry-tuned Li₂RuO₃ to the oxygen redox reaction involves the telescopic O-Ru-O configuration rather than O-O dimerization, which inhibits oxygen release, enabling significantly enhanced cycling stability and negligible voltage decay. This discovery of the new structural response mechanism for the oxygen redox reaction will provide a new scope for the strategy of enhancing the anionic redox stability, paving unexplored pathways toward further development of high capacity Li-rich layered oxides.

SUBMITTER: Ning F

PROVIDER: S-EPMC7532436 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Nanoparticles produced by bacteria, fungi, or plants generally have physicochemical properties such as size, shape, crystalline structure, magnetic properties, and stability which are difficult to obtain by chemical synthesis. For instance, Mn(II)-oxidizing organisms promote the biomineralization of manganese oxides with specific textures under ambient conditions. Controlling their crystallinity and texture may offer environmentally relevant routes of Mn oxide synthesis with potential technological applications, e.g., for energy storage. However, whereas the electrochemical activity of synthetic (abiotic) Mn oxides has been extensively studied, the electroactivity of Mn biominerals has been seldom investigated yet. Here we evaluated the electroactivity of biologically induced biominerals produced by the Mn(II)-oxidizer bacteria Pseudomonas putida strain MnB1. For this purpose, we explored the mechanisms of Mn biomineralization, including the kinetics of Mn(II) oxidation, under different conditions. Manganese speciation, biomineral structure, and texture as well as organic matter content were determined by a combination of X-ray diffraction, electron and X-ray microscopies, and thermogravimetric analyses coupled to mass spectrometry. Our results evidence the formation of an organic-inorganic composite material and a competition between the enzymatic (biotic) oxidation of Mn(II) to Mn(IV) yielding MnO2 birnessite and the abiotic formation of Mn(III), of which the ratio depends on oxygenation levels and activity of the bacteria. We reveal that a subtle control over the conditions of the microbial environment orients the birnessite to Mn(III)-phases ratio and the porosity of the assembly, which both strongly impact the bulk electroactivity of the composite biomineral. The electrochemical properties were tested in lithium battery configuration and exhibit very appealing performances (voltage, capacity, reversibility, and power capability), thanks to the specific texture resulting from the microbially driven synthesis route. Given that such electroactive Mn biominerals are widespread in the environment, our study opens an alternative route for the synthesis of performing electrode materials under environment-friendly conditions.

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Inhibition of oxygen dimerization by local symmetry tuning in Li-rich layered oxides for improved stability.

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