Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.341
Publication date: 18th December 2023
Lithium-ion (Li-ion) and Sodium-ion (Na-ion) batteries function through reversible intercalation reactions involving an intercalant cation (A = Li+ or Na+) into a host compound (AxH), which serves as the active material in the positive electrode (often referred to as the 'cathode'). These intercalation reactions generally occur through two distinct mechanisms:
(i) Homogeneous reactions, characterized by a single phase or solid solution, involves the formation of a non-stoichiometric compound (AxH) where the insertion content 'x' continuously varies within the intercalation domain xmin ≥ x ≥ xmax.
(ii) Heterogeneous reactions involve multi-phase processes, leading to the nucleation and growth of a second phase (AyH, where y ≠ x) as a results of the compositional changes within the electrode.
In single-phase reactions, the host structure undergoes minimal structural changes, primarily a continuous volume variation to accommodate the compositional shift. This is generally considered more favorable for fast diffusion compared to the moving interfaces found in two-phase reactions. However, the rate of intercalation reactions, (driven by the imposed rate of the charge and/or discharge processes) can lead electrodes away from equilibrium conditions. This departure can induce significant variations in reaction mechanisms, including changes in phase transition sequences.
This presentation will showcase how operando powder X-ray diffraction (XRD) and absorption spectroscopy (XAS) experiments offer valuable insights into the understanding of reaction mechanisms in electrode materials. Examples include Li-rich layered oxides [1], the high-voltage spinel LiNi0.5Mn1.5O4 [2], and Na-ion triphylite (olivine-type) cathode materials such as NaFePO4 and NaFe0.8Mn0.2PO4 [3,4].
The work presented in this talk has received funding support from the European Commission (EU H2020, project 3beLiEVe G.A. 875033), the Spanish MCIN/AEI/10.13039/50110001103 (projects ION-SELF ref. PID2019-106519RB-I00, NIB-MOVE ref. PID2019-107468RB-C22, AffINITy ref. ENE2016‐75242‐R), MCIN/AEI/10.13039/501100011033/ and EDRF A way of making Europe (project SMART ref. PID2022-137626OB-C33), Ministerio de Industria, Comercio y Turismo, funded by the European Union – Next Generation EU (project VEC-020100-2022-127/PP27) and the Basque Government (PhD grant ref. PRE-2021-2-011, Elkartek programs CICe2017 and CICe2020). The authors are thankful for beamtime at ALBA synchrotron and the support received from the beamline staff: François Fauth (XRD, BL04-MSPD), Martin-Diaconescu and Laura Simonelli (XAS, BL22-CLAESS), Giovanni Agostini and Carlos Escudero (XAS, BL16-NOTOS)
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