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Entropy and crystal-facet modulation of P2-type layered cathodes for long-lasting sodium-based batteries.

ABSTRACT: P2-type sodium manganese-rich layered oxides are promising cathode candidates for sodium-based batteries because of their appealing cost-effective and capacity features. However, the structural distortion and cationic rearrangement induced by irreversible phase transition and anionic redox reaction at high cell voltage (i.e., >4.0 V) cause sluggish Na-ion kinetics and severe capacity decay. To circumvent these issues, here, we report a strategy to develop P2-type layered cathodes via configurational entropy and ion-diffusion structural tuning. In situ synchrotron X-ray diffraction combined with electrochemical kinetic tests and microstructural characterizations reveal that the entropy-tuned Na_0.62Mn_0.67Ni_0.23Cu_0.05Mg_0.07Ti_0.01O₂ (CuMgTi-571) cathode possesses more {010} active facet, improved structural and thermal stability and faster anionic redox kinetics compared to Na_0.62Mn_0.67Ni_0.37O₂. When tested in combination with a Na metal anode and a non-aqueous NaClO₄-based electrolyte solution in coin cell configuration, the CuMgTi-571-based positive electrode enables an 87% capacity retention after 500 cycles at 120 mA g^-1 and about 75% capacity retention after 2000 cycles at 1.2 A g^-1.

SUBMITTER: Fu F

PROVIDER: S-EPMC9123165 | biostudies-literature | 2022 May

REPOSITORIES: biostudies-literature

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Entropy and crystal-facet modulation of P2-type layered cathodes for long-lasting sodium-based batteries.

Fu Fang F Liu Xiang X Fu Xiaoguang X Chen Hongwei H Huang Ling L Fan Jingjing J Le Jiabo J Wang Qiuxiang Q Yang Weihua W Ren Yang Y Amine Khalil K Sun Shi-Gang SG Xu Gui-Liang GL

Nature communications 20220520 1

P2-type sodium manganese-rich layered oxides are promising cathode candidates for sodium-based batteries because of their appealing cost-effective and capacity features. However, the structural distortion and cationic rearrangement induced by irreversible phase transition and anionic redox reaction at high cell voltage (i.e., >4.0 V) cause sluggish Na-ion kinetics and severe capacity decay. To circumvent these issues, here, we report a strategy to develop P2-type layered cathodes via configurati ...[more]

PMID: 35595772

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Project description:ConspectusLithium-ion batteries (LIBs) are ubiquitous in all modern portable electronic devices such as mobile phones and laptops as well as for powering hybrid electric vehicles and other large-scale devices. Sodium-ion batteries (NIBs), which possess a similar cell configuration and working mechanism, have already been proven as ideal alternatives for large-scale energy storage systems. The advantages of NIBs are as follows. First, sodium resources are abundantly distributed in the earth's crust. Second, high-performance NIB cathode materials can be fabricated by using solely inexpensive and noncritical transition metals such as manganese and iron, which further reduces the cost of the required raw materials. Recently, the unprecedented demand for lithium and other critical minerals has driven the cost of these primary raw materials (which are utilized in LIBs) to a historic high and thus triggered the commercialization of NIBs.Sodium layered transition metal oxides (NaxTMO2, TM = transition metal/s), such as Mn-based sodium layered oxides, represent an important family of cathode materials with the potential to reduce costs, increase energy density and cycling stability, and improve the safety of NIBs for large-scale energy storage. However, these layered oxides face several key challenges, including irreversible phase transformations during cycling, poor air stability, complex charge-compensation mechanisms, and relatively high cost of the full cell compared to LiFePO4-based LIBs. Our work has focused on the techno-economic analysis, the degradation mechanism of NaxTMO2 upon cycling and air exposure, and the development of effective strategies to improve their electrochemical performances and air stability. Correlating structure-performance relationships and establishing general design strategies of NaxTMO2 must be considered for the commercialization of NIBs.In this Account, we discuss the recent progress in the development of air-stable, electrochemically stable, and cost-effective NaxTMO2. The favorable redox-active cations for NaxTMO2 are emphasized in terms of abundance, cost, supply, and energy density. Different working mechanisms related to NaxTMO2 are summarized, including the electrochemical reversibility, the main structural transformations during the charge and discharge processes, and the charge-compensation mechanisms that accompany the (de)intercalation of Na+ ions, followed by discussions to improve the stability toward ambient air and upon cycling. Then the techno-economics are presented, with an emphasis on cathodes with different chemical compositions, cost breakdown of battery packs, and Na deficiency, factors that are critical to the large-scale implementation. Finally, this Account concludes with an overview of the remaining challenges and new opportunities concerning the practical applications of NaxTMO2, with an emphasis on the cost, large-scale fabrication capability, and electrochemical performance.

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Entropy and crystal-facet modulation of P2-type layered cathodes for long-lasting sodium-based batteries.

Publications

Entropy and crystal-facet modulation of P2-type layered cathodes for long-lasting sodium-based batteries.

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