Enhanced electrochemical performance of manganese-based metal organic frameworks-derived spinel LiMn2O4 cathode materials by improving the Mn3+ content and oxygen vacancies

Chen, Ziliang; Gu, Yijing; Huo, Yong-Lin; Ma, Xiao-Yu; Wu, Fuzhong

doi:10.1016/j.jallcom.2022.165485

Cited by 25 publications

(23 citation statements)

References 50 publications

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“…The button battery was kept in an air-conditioned space to maintain a constant temperature, but sudden changes in the outside temperature still caused minor variations in the data. This type of variation is typical, and it has also appeared in many reported documents. , Figure b compares the electrochemical capabilities of recently developed LLOs; for details, see Table S6. ,,,− Although the number of cycles is different, the capacity retention rates of materials in these documents are quite excellent. A major obstacle to the commercialization of batteries is the voltage decay of LLOs.…”

Section: Resultssupporting

confidence: 58%

“…The corresponding fitting images and data are provided in Figure S1 and Table S2. The R values R p and R wp of all the samples are less than 5%, and the χ of all the samples is between 1 and 1.3, which indicates that the Rietveld refinement result is reliable . Obviously, the lattice parameters “ a ” and “ c ” decrease after Al doping.…”

Section: Resultsmentioning

confidence: 87%

“…Figure b shows the CV experiments of the LRM, LRMA, and 3@LRMA electrodes in the range of 0.1–1 mV, which were performed to further investigate the effect of Al doping and DH coating on lithium-ion diffusion kinetics. The Li-ion diffusion coefficient is calculated according to Note S1 . Based on Note S1, the data were fitted in a straight line that reflects the D Li value, as shown in Figure b.…”

Section: Resultsmentioning

confidence: 99%

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Inhibition of Structural Transformation and Surface Lattice Oxygen Activity for Excellent Stability Li-Rich Mn-Based Layered Oxides

Huo

Chen

et al. 2023

ACS Appl. Mater. Interfaces

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Li-rich Mn-based layered oxides (LLOs) are one of the most promising cathode materials, which have exceptional anionic redox activity and a capacity that surpasses 250 mA h/g. However, the change from a layered structure to a spinel structure and unstable anionic redox are accompanied by voltage attenuation, poor rate performance, and problematic capacity. The technique of stabilizing the crystal structure and reducing the surface oxygen activity is proposed in this paper. A coating layer and highly concentrated oxygen vacancies are developed on the material’s surface, according to scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. In situ EIS shows that structural transformation and oxygen release are inhibited during the first charge and discharge. Optimized 3@LRMA has an average attenuation voltage of 0.55 mV per cycle (vs 1.7 mV) and a capacity retention rate of 93.4% after 200 cycles (vs 52.8%). Postmortem analysis indicates that the successful doping of Al ions into the crystal structure effectively inhibits the structural alteration of the cycling process. The addition of oxygen vacancies reduces the surface lattice’s redox activity. Additionally, surface structure deterioration is successfully halted by N- and Cl-doped carbon coating. This finding highlights the significance of lowering the surface lattice oxygen activity and preventing structural alteration, and it offers a workable solution to increase the LLO stability.

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Section: Resultssupporting

confidence: 58%

Section: Resultsmentioning

confidence: 87%

Section: Resultsmentioning

confidence: 99%

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Inhibition of Structural Transformation and Surface Lattice Oxygen Activity for Excellent Stability Li-Rich Mn-Based Layered Oxides

Huo

Chen

et al. 2023

ACS Appl. Mater. Interfaces

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“…The intensity ratios were calculated (Table 1) for all samples to compare the crystal structure plane orientations. The I (111) /I (311) ratios showed similar values, with values of 1.88 for LMO-W and 1.81 for LMO-E and LMO-G; however, the value for the LMO-W sample being slightly higher indicates that the powder had a preferential orientation along the (111) crystallographic direction [37][38][39][40]. The (111) crystal planes of the spinel LMO particles being predominantly oriented in a particular direction can lead to anisotropic properties, such as different electrochemical performances in different crystallographic directions.…”

Section: Structure and Morphologymentioning

confidence: 85%

“…If the sol-gel matrix is not properly removed during calcination, it can leave behind carbonaceous residues that could interfere with the formation of the spinel phase or affect its properties [24]; therefore, carbonaceous residues were completely removed by calcinating the samples at 800 • C, as reported in the literature [24], which was confirmed by the XRD results. The intensity ratios I (111) /I (311) , I (311) /I (400) , I (400) /I (111) , and I (440) /I (111) from the crystal facet XRD patterns of spinel LMO powder provide information about the crystal structure and orientation of the material [37]; the I (111) /I (311) ratio indicates the growth of the (111) crystal plane, whereas the (440) and (400) crystal facets correspond to the (110) and (100) crystal planes, respectively [37]. The intensity ratios were calculated (Table 1) for all samples to compare the crystal structure plane orientations.…”

Section: Structure and Morphologymentioning

confidence: 99%

Unraveling the Mechanism and Practical Implications of the Sol-Gel Synthesis of Spinel LiMn2O4 as a Cathode Material for Li-Ion Batteries: Critical Effects of Cation Distribution at the Matrix Level

et al. 2023

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Spinel LiMn2O4 (LMO) is a state-of-the-art cathode material for Li-ion batteries. However, the operating voltage and battery life of spinel LMO needs to be improved for application in various modern technologies. Modifying the composition of the spinel LMO material alters its electronic structure, thereby increasing its operating voltage. Additionally, modifying the microstructure of the spinel LMO by controlling the size and distribution of the particles can improve its electrochemical properties. In this study, we elucidate the sol-gel synthesis mechanisms of two common types of sol-gels (modified and unmodified metal complexes)—chelate gel and organic polymeric gel—and investigate their structural and morphological properties and electrochemical performances. This study highlights that uniform distribution of cations during sol-gel formation is important for the growth of LMO crystals. Furthermore, a homogeneous multicomponent sol-gel, necessary to ensure that no conflicting morphologies and structures would degrade the electrochemical performances, can be obtained when the sol-gel has a polymer-like structure and uniformly bound ions; this can be achieved by using additional multifunctional reagents, namely cross-linkers.

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Regulating the Manganese Valence State Improves the Kinetic Properties of Manganese‐Based Cathodes

Zhang,

Yuan,

Qin

et al. 2024

Adv Funct Materials

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Manganese (Mn)‐based lithium (Li)‐ion batteries with high energy density and low cost have recently attracted considerable attention. One drawback of Mn‐based batteries is the severe capacity attenuation caused by the Jahn‐Teller effect, which distorts the crystal structure and reduces the kinetics of Li‐ion insertion/extraction in the cathodes. In this study, the Mn valence state is regulated on the surface of Mn‐based oxide particles and oxygen vacancies are introduced to facilitate rapid Li‐ion transport and charge storage by adding succinonitrile (SN) to Mn‐based cathodes. Because of the reaction between SN and Mn‐based cathode particles, the contents of Mn3+ ions and oxygen vacancies increase, leading to an improvement in the Li‐ion kinetic properties of the cathodes as well as a reduction in the dissolution of Mn from the cathodes. By regulating the Mn valence state, Li‐ion and Li metal batteries with LiMn2O4 or Li‐rich Mn‐based layered oxide cathodes show significantly enhanced discharge capacity and improved cyclic performance. This study demonstrates that regulating the valence state of Mn ions is an effective strategy for enhancing the electrochemical performance of Mn‐based Li batteries and that adding SN to the cathodes is a cost‐effective method for mass production.

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Enhanced electrochemical performance of manganese-based metal organic frameworks-derived spinel LiMn2O4 cathode materials by improving the Mn3+ content and oxygen vacancies

Cited by 25 publications

References 50 publications

Inhibition of Structural Transformation and Surface Lattice Oxygen Activity for Excellent Stability Li-Rich Mn-Based Layered Oxides

Inhibition of Structural Transformation and Surface Lattice Oxygen Activity for Excellent Stability Li-Rich Mn-Based Layered Oxides

Unraveling the Mechanism and Practical Implications of the Sol-Gel Synthesis of Spinel LiMn2O4 as a Cathode Material for Li-Ion Batteries: Critical Effects of Cation Distribution at the Matrix Level

Regulating the Manganese Valence State Improves the Kinetic Properties of Manganese‐Based Cathodes

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