| 1. |
- Pereira de Carvalho, Rodrigo, et al.
(författare)
-
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
- 2021
-
Ingår i: Materials Advances. - : Royal Society of Chemistry. - 2633-5409. ; 2:3, s. 1024-1034
-
Tidskriftsartikel (refereegranskat)abstract
- 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+.
|
|
| 2. |
|
|
| 3. |
- Oltean, Viorica Alina, et al.
(författare)
-
Enhanced performance of organic materials for lithium-ion batteries using facile electrode calendaring techniques
- 2016
-
Ingår i: Electrochemistry communications. - : Elsevier BV. - 1388-2481 .- 1873-1902. ; 68, s. 45-48
-
Tidskriftsartikel (refereegranskat)abstract
- A simple and convenient strategy for achieving higher capacities in organic electrode materials used in pouch-cell format is presented here. By calendaring of the electrodes, the resulting electrode porosity can be tailored. It is shown for carboxylate electrodes of dilithium benzenediacrylate that a 30% porosity constitutes the best compromise between electronic wiring, particle contact and electrolyte infiltration into the electrodes, displaying higher capacities than in Swagelock cells.
|
|
| 4. |
|
|
| 5. |
- Oltean, Viorica Alina, et al.
(författare)
-
Investigating the Interfacial Chemistry of Organic Electrodes in Li- and Na-Ion Batteries
- 2016
-
Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 28:23, s. 8742-8751
-
Tidskriftsartikel (refereegranskat)abstract
- Organic compounds are increasingly being investigated as electrode materials for Li- or Na-ion batteries. Even though their gravimetric capacity can challenge that of their inorganic counterparts, a number of problems need further attention, not least their chemical and electrochemical stability toward the electrolyte systems. There has been speculation that several of these issues have their origin in the formation of a less stable solid electrolyte interphase (SEI) layer and its evolution during battery cycling. We here present the very first thorough characterization of the organic electrode material SEI layer using hard X-ray photoelectron spectroscopy (HAXPES), for both Li- and Na-based electrodes. Dilithium and disodium benzenediacrylates have been used for battery construction and investigated electrochemically followed by HAXPES measurements electrolyte and after cycling. The Na-based electrodes react spontaneously with the electrolyte, and the SEI layer is dominated by inorganic species with continuous salt degradation during cycling. The Li-based electrodes display an SEI layer with primarily organic species from solvent degradation products appearing only after cycling and increasing in amount with the number of electrochemical cycles.
|
|
| 6. |
- Oltean, Viorica-Alina, et al.
(författare)
-
Sustainable Materials for Sustainable Energy Storage : Organic Na Electrodes
- 2016
-
Ingår i: Materials. - : MDPI AG. - 1996-1944. ; 9:3
-
Forskningsöversikt (refereegranskat)abstract
- In this review, we summarize research efforts to realize Na-based organic materials for novel battery chemistries. Na is a more abundant element than Li, thereby contributing to less costly materials with limited to no geopolitical constraints while organic electrode materials harvested from biomass resources provide the possibility of achieving renewable battery components with low environmental impact during processing and recycling. Together, this can form the basis for truly sustainable electrochemical energy storage. We explore the efforts made on electrode materials of organic salts, primarily carbonyl compounds but also Schiff bases, unsaturated compounds, nitroxides and polymers. Moreover, sodiated carbonaceous materials derived from biomasses and waste products are surveyed. As a conclusion to the review, some shortcomings of the currently investigated materials are highlighted together with the major limitations for future development in this field. Finally, routes to move forward in this direction are suggested.
|
|
| 7. |
- Renault, Stevén, et al.
(författare)
-
Dilithium 2-aminoterephthalate as a negative electrode material for lithium-ion batteries
- 2017
-
Ingår i: Solid State Ionics. - : Elsevier BV. - 0167-2738 .- 1872-7689. ; 307, s. 1-5
-
Tidskriftsartikel (refereegranskat)abstract
- This work presents the synthesis and characterization of a novel organic Li-battery anode material: dilithium 2-aminoterephthalate (C8H5Li2NO4). When investigated in Li half-cells, the resulting electrodes show stable capacities around ca. 180 mAh g− 1 and promising rate capabilities, with battery performance at 500 mA g− 1 and good capacity recovery, despite being an asymmetric compound. DFT calculations indicate a preferential lithiation on carboxylates close to the amino group.
|
|
| 8. |
|
|
| 9. |
|
|
| 10. |
- Renault, Stéven, et al.
(författare)
-
Superlithiation of Organic Electrode Materials : The Case of Dilithium Benzenedipropiolate
- 2016
-
Ingår i: Chemistry of Materials. - : American Chemical Society (ACS). - 0897-4756 .- 1520-5002. ; 28:6, s. 1920-1926
-
Tidskriftsartikel (refereegranskat)abstract
- Dilithium benzenedipropiolate was prepared and investigated as a potential negative electrode material for secondary lithium-ion batteries. In addition to the expected reduction of its carbonyls, this material can reduce and reversibly oxidize its unsaturated carbon–carbon bonds leading to a Li/C ratio of 1/1 and a specific capacity as high as 1363 mAh g–1: the highest ever reported for a lithium carboxylate. Density functional theory calculations suggest that the lithiation is preferential on the propiolate carbons.
|
|
