Structure–property relationships in organic battery anode materials: exploring redox reactions in crystalline Na- and Li-benzene diacrylate using combined crystallography and density functional theory calculations
| العنوان: | Structure–property relationships in organic battery anode materials: exploring redox reactions in crystalline Na- and Li-benzene diacrylate using combined crystallography and density functional theory calculations |
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| المؤلفون: | Rodrigo P. Carvalho, Viorica-Alina Oltean, Daniel Brandell, Cesar Pay Gómez, C. Moyses Araujo, Cleber F. N. Marchiori, Tom Willhammar, Stéven Renault |
| المساهمون: | Uppsala University, Institut des Matériaux Jean Rouxel (IMN), Université de Nantes - UFR des Sciences et des Techniques (UN UFR ST), Université de Nantes (UN)-Université de Nantes (UN)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Ecole Polytechnique de l'Université de Nantes (EPUN), Université de Nantes (UN)-Université de Nantes (UN), Stockholm University, Karlstad University [Sweden] |
| المصدر: | Materials Advances Materials Advances, Royal Society of Chemistry, 2021, 2 (3), pp.1024-1034. ⟨10.1039/d0ma00900h⟩ |
| بيانات النشر: | HAL CCSD, 2021. |
| سنة النشر: | 2021 |
| مصطلحات موضوعية: | Battery (electricity), Oorganisk kemi, Materials science, Materialkemi, Organic radical battery, Disproportionation, 02 engineering and technology, Crystal structure, 010402 general chemistry, 021001 nanoscience & nanotechnology, Electrochemistry, Condensed Matter Physics, 01 natural sciences, 0104 chemical sciences, Inorganic Chemistry, Electron diffraction, Chemistry (miscellaneous), Materials Chemistry, [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci], Physical chemistry, General Materials Science, Density functional theory, 0210 nano-technology, Single crystal, Den kondenserade materiens fysik |
| الوصف: | Organic-based materials are potential candidates for a new generation of sustainable and environmentally friendly battery technologies, but insights into the structural, kinetic and thermodynamic properties of how these compounds lithiate or sodiate are currently missing. In this regard, benzenediacrylates (BDAs) are here investigated for application as low-potential electrodes in Na-ion and Li-ion batteries. Aided by a joint effort of theoretical and experimental frameworks, we unveil the structural, electronic and electrochemical properties of the Na(2)BDA and Li(2)BDA compounds. The crystal structure of these systems in their different sodiated and lithiated phases have been predicted by an evolutionary algorithm interplayed with density functional theory calculations. Due to difficulties in obtaining useful single crystals for the BDA salts, other methods have been explored in combination with the computational approach. While the predicted structure of the pristine Na(2)BDA compound has been experimentally confirmed through the 3D Electron Diffraction (3DED) technique, the hydrated version of Li(2)BDA is analysed through single crystal X-ray diffraction. The calculated cell voltages for the sodiation (0.63 V vs. Na/Na+) and lithiation (1.12 V vs. Li/Li+) processes display excellent quantitative agreement with experimental findings. These results validate the developed theoretical methodology. Moreover, fundamental aspects of the electronic structures and their relationship with the reaction thermodynamics are discussed. The results suggest a possible disproportionation between the sodiated phases of Na(2)BDA, supporting a two-electron process, and also unveil major differences for the two employed cations: Na+ and Li+. |
| وصف الملف: | application/pdf |
| اللغة: | English |
| تدمد: | 2633-5409 |
| DOI: | 10.1039/d0ma00900h⟩ |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::d39bcae9663571f07ac2a3839a388069 https://hal.archives-ouvertes.fr/hal-03266195 |
| Rights: | OPEN |
| رقم الانضمام: | edsair.doi.dedup.....d39bcae9663571f07ac2a3839a388069 |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 26335409 |
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| DOI: | 10.1039/d0ma00900h⟩ |