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A Bifunctional-Modulated Conformal Li/Mn-Rich Layered Cathode for Fast-Charging, High Volumetric Density and Durable Li-Ion Full Cells.

ABSTRACT: Lithium- and manganese-rich (LMR) layered cathode materials hold the great promise in designing the next-generation high energy density lithium ion batteries. However, due to the severe surface phase transformation and structure collapse, stabilizing LMR to suppress capacity fade has been a critical challenge. Here, a bifunctional strategy that integrates the advantages of surface modification and structural design is proposed to address the above issues. A model compound Li_1.2Mn_0.54Ni_0.13Co_0.13O₂ (MNC) with semi-hollow microsphere structure is synthesized, of which the surface is modified by surface-treated layer and graphene/carbon nanotube dual layers. The unique structure design enabled high tap density (2.1 g cm^-3) and bidirectional ion diffusion pathways. The dual surface coatings covalent bonded with MNC via C-O-M linkage greatly improves charge transfer efficiency and mitigates electrode degradation. Owing to the synergistic effect, the obtained MNC cathode is highly conformal with durable structure integrity, exhibiting high volumetric energy density (2234 Wh L^-1) and predominant capacitive behavior. The assembled full cell, with nanographite as the anode, reveals an energy density of 526.5 Wh kg^-1, good rate performance (70.3% retention at 20 C) and long cycle life (1000 cycles). The strategy presented in this work may shed light on designing other high-performance energy devices.

SUBMITTER: Zhao Z

PROVIDER: S-EPMC8089071 | 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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A Bifunctional-Modulated Conformal Li/Mn-Rich Layered Cathode for Fast-Charging, High Volumetric Density and Durable Li-Ion Full Cells.

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