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Operando acoustic emission monitoring of degradation processes in lithium-ion batteries with a high-entropy oxide anode.

ABSTRACT: In recent years, high-entropy oxides are receiving increasing attention for electrochemical energy-storage applications. Among them, the rocksalt (Co_0.2Cu_0.2Mg_0.2Ni_0.2Zn_0.2)O (HEO) has been shown to be a promising high-capacity anode material. Because high-entropy oxides constitute a new class of electrode materials, systematic understanding of their behavior during ion insertion and extraction is yet to be established. Here, we probe the conversion-type HEO material in lithium half-cells by acoustic emission (AE) monitoring. Especially the clustering of AE signals allows for correlations of acoustic events with various processes. The initial cycle was found to be the most acoustically active because of solid-electrolyte interphase formation and chemo-mechanical degradation. In the subsequent cycles, AE was mainly detected during delithiation, a finding we attribute to the progressive crack formation and propagation. Overall, the data confirm that the AE technology as a non-destructive operando technique holds promise for gaining insight into the degradation processes occurring in battery cells during cycling.

SUBMITTER: Schweidler S

PROVIDER: S-EPMC8642430 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Lithiation Mechanism in High-Entropy Oxides as Anode Materials for Li-Ion Batteries: An Operando XAS Study.

Project description:High-entropy oxides based on transition metals, such as Mg0.2Co0.2Ni0.2Cu0.2Zn0.2O (TM-HEO), have recently drawn special attention as potential anodes in lithium-ion batteries due to high specific capacity and cycling reversibility. However, the lithiation/delithiation mechanism of such systems is still controversial and not clearly addressed. Here, we report on an operando XAS investigation into TM-HEO-based anodes for lithium-ion cells during the first lithiation/delithiation cycle. This material showed a high specific capacity exceeding 600 mAh g-1 at 0.1 C and Coulombic efficiency very close to unity. The combination of functional and advanced spectroscopic studies revealed complex charging mechanisms, developing through the reduction of transition-metal (TM) cations, which triggers the conversion reaction below 1.0 V. The conversion is irreversible and incomplete, leading to the final collapse of the HEO rock-salt structure. Other redox processes are therefore discussed and called to account for the observed cycling behavior of the TM-HEO-based anode. Despite the irreversible phenomena, the HEO cubic structure remains intact for ∼60% of lithiation capacity, so proving the beneficial role of the configuration entropy in enhancing the stability of the HEO rock-salt structure during the redox phenomena.

| S-EPMC8016163 | biostudies-literature

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| S-EPMC7359355 | biostudies-literature

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| S-EPMC5080607 | biostudies-literature

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| S-EPMC3884641 | biostudies-literature

Defective Ti2Nb10O27.1: an advanced anode material for lithium-ion batteries.

Project description:To explore anode materials with large capacities and high rate performances for the lithium-ion batteries of electric vehicles, defective Ti2Nb10O27.1 has been prepared through a facile solid-state reaction in argon. X-ray diffractions combined with Rietveld refinements indicate that Ti2Nb10O27.1 has the same crystal structure with stoichiometric Ti2Nb10O29 (Wadsley-Roth shear structure with A2/m space group) but larger lattice parameters and 6.6% O(2-) vacancies (vs. all O(2-) ions). The electronic conductivity and Li(+)ion diffusion coefficient of Ti2Nb10O27.1 are at least six orders of magnitude and ~2.5 times larger than those of Ti2Nb10O29, respectively. First-principles calculations reveal that the significantly enhanced electronic conductivity is attributed to the formation of impurity bands in Ti2Nb10O29-x and its conductor characteristic. As a result of the improvements in the electronic and ionic conductivities, Ti2Nb10O27.1 exhibits not only a large initial discharge capacity of 329 mAh g(-1) and charge capacity of 286 mAh g(-1) at 0.1 C but also an outstanding rate performance and cyclability. At 5 C, its charge capacity remains 180 mAh g(-1) with large capacity retention of 91.0% after 100 cycles, whereas those of Ti2Nb10O29 are only 90 mAh g(-1) and 74.7%.

| S-EPMC4668578 | biostudies-literature

Reaction Mechanism of the Sn2Fe Anode in Lithium-Ion Batteries.

Project description:Sn2Fe anode materials were synthesized by a solvothermal route, and their electrochemical performance and reaction mechanism were evaluated. The structural evolution in the first two lithium cycles was investigated by X-ray absorption spectroscopy (XAS), synchrotron X-ray diffraction (XRD), and magnetic studies. In the first cycle, progressive alloying of Sn with Li accompanied by metallic iron displacement occurs upon lithiation, and the delithiation proceeds by Li x Sn dealloying and recovery of the Sn2Fe phase. In the second cycle, both XRD and XAS identify Li-Sn alloying at earlier lithiation stages than in the first cycle, with low-Li-content alloys evident in the beginning of the lithiation process. In the fully lithiated state, XAS analysis reveals higher coordination numbers in both the Li x Sn and Fe phases, which points toward more complete reaction and higher crystallinity of the products. Upon second delithiation, the Sn2Fe phase is generally reformed as evidenced by XRD. However, XAS indicates somewhat reduced Sn-Fe coordination and shorter Fe-Fe distance, which indicates incomplete reconversion and metallic Fe retention, which is also evident in the magnetic studies. Thus, a combination of long-range (XRD, magnetic) and local (XAS) techniques has revealed differences between the first and the second Li cycles relevant to the understanding of the capacity fading mechanisms.

| S-EPMC6941190 | biostudies-literature

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Project description:This work describes a potential anode material for lithium-ion batteries (LIBs), namely, anatase TiO2 nanoparticle-decorated carbon nanotubes (CNTs@TiO2). The electrochemical properties of CNTs@TiO2 were thoroughly investigated using various electrochemical techniques, including cyclic voltammetry, electrochemical impedance spectroscopy, galvanostatic cycling, and rate experiments. It was revealed that compared with pure TiO2 nanoparticles and CNTs alone, the CNT@TiO2 nanohybrids offered superior rate capability and achieved better cycling performance when used as anodes of LIBs. The CNT@TiO2 nanohybrids exhibited a cycling stability with high reversible capacity of about 190 mAh g-1 after 120 cycles at a current density of 100 mA g-1 and an excellent rate capability (up to 100 mAh g-1 at a current density of 1,000 mA g-1).

| S-EPMC3874633 | biostudies-literature

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| S-EPMC4350083 | biostudies-literature

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| S-EPMC7288579 | biostudies-literature

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