Solvation chemistry of electrolytes for stable anodes of lithium metal batteries

Huang, Yaohui; Wen, Bo; Jiang, Zhuoliang; Li, Fujun

doi:10.1007/s12274-022-4839-8

Cited by 25 publications

(19 citation statements)

References 89 publications

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“…The variation in charges on the dissociated atoms are also shown in Figure S8(b-e). The decomposition of salt molecules when present in high concentration supports the fact that, with increase in concentration, there are higher chances for salt anions to participate in the solvation shells around cations thereby making the anion reduction easier as explained in various reports. , The atomic F anions are found to adsorb on the Al surface mostly. The salt decompositions are found to take place before the EC solvent reduction.…”

Section: Resultssupporting

confidence: 58%

“…On one hand, SEI formation requires the decomposition of various electrolyte components, a robust SEI once formed restricts further direct contact between the electrode and electrolyte thereby obstructing further electrolyte decomposition which can positively contribute to the longevity of the battery . In various reports, it has been proposed that an inorganic-rich SEI layer is recommended as it is robust and stops dendrite formation. , The organic rich SEI on the other hand leads to low ionic conductivity in the battery . Among the considered salts (LiPF 6 , LiBF 4 , and LiTFSI) in our study, LiBF 4 is found to have the least tendency to participate in SEI formation.…”

Section: Resultsmentioning

confidence: 88%

“…The decomposition of salt molecules when present in high concentration supports the fact that, with increase in concentration, there are higher chances for salt anions to participate in the solvation shells around cations thereby making the anion reduction easier as explained in various reports. 21,45 The atomic F anions are found to adsorb on the Al surface mostly. The salt decompositions are found to Interestingly, in the case of the LiAl surface, only one of the four LiPF 6 salts is found to decompose (Figure 4(b) and Figure S9(a)).…”

Section: M Lipf 6 In Ecmentioning

confidence: 99%

“…19,20 Low salt concentration in the electrolyte leads to organic-rich SEI, whereas higher salt concentrations are expected to result in an inorganic-rich SEI. 21 The competition between the reduction of salt or the solvent is largely decided by their competitive participation in the solvation shell. Various studies have shown that the salt decomposition is more probable in the case of a contact ion pair model where the cation and anion of the salt are in the same solvation shell.…”

Section: Introductionmentioning

confidence: 99%

“…The SEI composition is also found to affect the battery performance. If the SEI is majorly composed of organic components from the solvent, the SEI flexibility is improved helping in tolerating volume change but leading to high interfacial resistance and sluggish dynamic kinetics. , On the other hand, an SEI composed of inorganic components from the anions lead to an SEI with high ionic conductivity. , Low salt concentration in the electrolyte leads to organic-rich SEI, whereas higher salt concentrations are expected to result in an inorganic-rich SEI . The competition between the reduction of salt or the solvent is largely decided by their competitive participation in the solvation shell.…”

Section: Introductionmentioning

confidence: 99%

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Suitable Salt for Solid Electrolyte Interphase Formation in Al Anode Dual-Ion Battery

Das

Pathak

2023

ACS Appl. Energy Mater.

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Solid electrolyte interphase (SEI) formation upon reaction between electrode and electrolyte is an important phenomenon in metal anode-based batteries. Various components such as the nature of the electrode surface, solvent, additive, and salt contribute toward the SEI formation. In this work, we carried out ab initio molecular dynamics (AIMD) simulations on an electrolyte involving three different salts (LiPF6, LiBF4, and LiTFSI) in contact with the Al and LiAl anodes. We also checked the role played by the concentration of salt along with its nature during SEI formation. Different extents of salt decomposition are identified in different cases, and LiTFSI is found to be the most suitable salt leading to an inorganic-component-rich SEI layer. LiBF4 on the other hand decomposes minimally resulting in a solvent derived organic SEI. We highlight the importance of preferential reduction of salt before solvent to form inorganic-rich SEI which is preferable compared to organic SEI. The higher salt concentration is also found to support preferential salt decomposition. Overall, our work signifies the choice of proper salt along with its concentration to tune the SEI growth process in Al anode dual-ion batteries.

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Section: Resultssupporting

confidence: 58%

Section: Resultsmentioning

confidence: 88%

Section: M Lipf 6 In Ecmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Suitable Salt for Solid Electrolyte Interphase Formation in Al Anode Dual-Ion Battery

Das

Pathak

2023

ACS Appl. Energy Mater.

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Solvation Regulation Reinforces Anion‐Derived Inorganic‐Rich Interphase for High‐Performance Quasi‐Solid‐State Li Metal Batteries

Xu,

Gao,

Huang

et al. 2024

Advanced Materials

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Solid‐state polymer lithium metal batteries are an important strategy for achieving high safety and high energy density. However, the issue of Li dendrites and inherent inferior interface greatly restricts practical application. Herein, this study introduces tris(2,2,2‐trifluoroethyl)phosphate solvent with moderate solvation ability, which can not only complex with Li+ to promote the in‐situ ring‐opening polymerization of 1,3‐dioxolane (DOL), but also build solvated structure models to explore the effect of different solvation structures in the polymer electrolyte. Thereinto, it is dominated by the contact ion pair solvated structure with pDOL chain segments forming less lithium bonds, exhibiting faster kinetic process and constructing a robust anion‐derived inorganic‐rich interphase, which significantly improves the utilization rate of active Li and the high‐voltage resistance of pDOL. As a result, it exhibits stable cycling at ultra‐high areal capacity of 20 mAh cm−2 in half cells, and an ultra‐long lifetime of over 2000 h in symmetric cells can be realized. Furthermore, matched with LiNi0.9Co0.05Mn0.05O2 cathode, the capacity retention after 60 cycles is as high as 96.8% at N/P value of 3.33. Remarkably, 0.7 Ah Li||LiNi0.9Co0.05Mn0.05O2 pouch cell with an energy density of 461 Wh kg−1 can be stably cycled for five cycles at 100% depth of discharge.

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Solvation Structure with Enhanced Anionic Coordination for Stable Anodes in Lithium‐Oxygen Batteries

et al. 2023

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Li‐O2 batteries have garnered much attention due to their high theoretical energy density. However, the irreversible lithium plating/stripping on the anode limits their performance, which has been paid little attention. Herein, a solvation‐regulated strategy for stable lithium anodes in tetraethylene glycol dimethyl ether (G4) based electrolyte is attempted in Li‐O2 batteries. Trifluoroacetate anions (TFA−) with strong Li+ affinity are incorporated into the lithium bis(fluorosulfonyl)imide (LiTFSI)/G4 electrolyte to attenuate the Li+‐G4 interaction and form anion‐dominant solvates. The bisalt electrolyte with 0.5 M LiTFA and 0.5 M LiTFSI mitigates G4 decomposition and induces an inorganic‐rich solid electrolyte interphase (SEI). This contributes to decreased desolvation energy barrier from 58.20 to 46.31 kJ mol−1, compared with 1.0 M LiTFSI/G4, for facile interfacial Li+ diffusion and high efficiency. It yields extended lifespan of 120 cycles in Li‐O2 battery with a limited Li anode (7 mAh cm−2). This work gains comprehensive insights into rational electrolyte design for Li‐O2 batteries.

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Solvation chemistry of electrolytes for stable anodes of lithium metal batteries

Cited by 25 publications

References 89 publications

Suitable Salt for Solid Electrolyte Interphase Formation in Al Anode Dual-Ion Battery

Suitable Salt for Solid Electrolyte Interphase Formation in Al Anode Dual-Ion Battery

Solvation Regulation Reinforces Anion‐Derived Inorganic‐Rich Interphase for High‐Performance Quasi‐Solid‐State Li Metal Batteries

Solvation Structure with Enhanced Anionic Coordination for Stable Anodes in Lithium‐Oxygen Batteries

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