Browse
Submit Data
Databases
API
Help

Dataset Information

28 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Electrostatic Interaction Tailored Anion-Rich Solvation Sheath Stabilizing High-Voltage Lithium Metal Batteries.

ABSTRACT: Through tailoring interfacial chemistry, electrolyte engineering is a facile yet effective strategy for high-performance lithium (Li) metal batteries, where the solvation structure is critical for interfacial chemistry. Herein, the effect of electrostatic interaction on regulating an anion-rich solvation is firstly proposed. The moderate electrostatic interaction between anion and solvent promotes anion to enter the solvation sheath, inducing stable solid electrolyte interphase with fast Li⁺ transport kinetics on the anode. This as-designed electrolyte exhibits excellent compatibility with Li metal anode (a Li deposition/stripping Coulombic efficiency of 99.3%) and high-voltage LiCoO₂ cathode. Consequently, the 50 μm-thin Li||high-loading LiCoO₂ cells achieve significantly improved cycling performance under stringent conditions of high voltage over 4.5 V, lean electrolyte, and wide temperature range (- 20 to 60 °C). This work inspires a groundbreaking strategy to manipulate the solvation structure through regulating the interactions of solvent and anion for high-performance Li metal batteries.

SUBMITTER: Wu J

PROVIDER: S-EPMC9304530 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Stabilizing polymer electrolytes in high-voltage lithium batteries.

Project description:Electrochemical cells that utilize lithium and sodium anodes are under active study for their potential to enable high-energy batteries. Liquid and solid polymer electrolytes based on ether chemistry are among the most promising choices for rechargeable lithium and sodium batteries. However, uncontrolled anionic polymerization of these electrolytes at low anode potentials and oxidative degradation at working potentials of the most interesting cathode chemistries have led to a quite concession in the field that solid-state or flexible batteries based on polymer electrolytes can only be achieved in cells based on low- or moderate-voltage cathodes. Here, we show that cationic chain transfer agents can prevent degradation of ether electrolytes by arresting uncontrolled polymer growth at the anode. We also report that cathode electrolyte interphases composed of preformed anionic polymers and supramolecules provide a fundamental strategy for extending the high voltage stability of ether-based electrolytes to potentials well above conventionally accepted limits.

| S-EPMC6626095 | biostudies-literature

Fluorinated ether electrolyte with controlled solvation structure for high voltage lithium metal batteries.

Project description:The development of new solvents is imperative in lithium metal batteries due to the incompatibility of conventional carbonate and narrow electrochemical windows of ether-based electrolytes. Whereas the fluorinated ethers showed improved electrochemical stabilities, they can hardly solvate lithium ions. Thus, the challenge in electrolyte chemistry is to combine the high voltage stability of fluorinated ethers with high lithium ion solvation ability of ethers in a single molecule. Herein, we report a new solvent, 2,2-dimethoxy-4-(trifluoromethyl)-1,3-dioxolane (DTDL), combining a cyclic fluorinated ether with a linear ether segment to simultaneously achieve high voltage stability and tune lithium ion solvation ability and structure. High oxidation stability up to 5.5 V, large lithium ion transference number of 0.75 and stable Coulombic efficiency of 99.2% after 500 cycles proved the potential of DTDL in high-voltage lithium metal batteries. Furthermore, 20 μm thick lithium paired LiNi0.8Co0.1Mn0.1O2 full cell incorporating 2 M LiFSI-DTDL electrolyte retained 84% of the original capacity after 200 cycles at 0.5 C.

| S-EPMC9076822 | biostudies-literature

Role of inner solvation sheath within salt-solvent complexes in tailoring electrode/electrolyte interphases for lithium metal batteries.

Project description:Functional electrolyte is the key to stabilize the highly reductive lithium (Li) metal anode and the high-voltage cathode for long-life, high-energy-density rechargeable Li metal batteries (LMBs). However, fundamental mechanisms on the interactions between reactive electrodes and electrolytes are still not well understood. Recently localized high-concentration electrolytes (LHCEs) are emerging as a promising electrolyte design strategy for LMBs. Here, we use LHCEs as an ideal platform to investigate the fundamental correlation between the reactive characteristics of the inner solvation sheath on electrode surfaces due to their unique solvation structures. The effects of a series of LHCEs with model electrolyte solvents (carbonate, sulfone, phosphate, and ether) on the stability of high-voltage LMBs are systematically studied. The stabilities of electrodes in different LHCEs indicate the intrinsic synergistic effects between the salt and the solvent when they coexist on electrode surfaces. Experimental and theoretical analyses reveal an intriguing general rule that the strong interactions between the salt and the solvent in the inner solvation sheath promote their intermolecular proton/charge transfer reactions, which dictates the properties of the electrode/electrolyte interphases and thus the battery performances.

| S-EPMC7682554 | biostudies-literature

Stabilizing nickel-rich layered oxide cathodes by magnesium doping for rechargeable lithium-ion batteries.

Project description:Nickel-rich layered transition metal oxides are attractive cathode materials for rechargeable lithium-ion batteries but suffer from inherent structural and thermal instabilities that limit the deliverable capacity and cycling performance on charging to a cutoff voltage above 4.3 V. Here we report LiNi0.90Co0.07Mg0.03O2 as a stable cathode material. The obtained LiNi0.90Co0.07Mg0.03O2 microspheres exhibit high capacity (228.3 mA h g-1 at 0.1C) and remarkable cyclability (84.3% capacity retention after 300 cycles). Combined X-ray diffraction and Cs-corrected microscopy reveal that Mg doping stabilizes the layered structure by suppressing Li/Ni cation mixing and Ni migration to interlayer Li slabs. Because of the pillar effect of Mg in Li sites, LiNi0.90Co0.07Mg0.03O2 shows decent thermal stability and small lattice variation until it is charged to 4.7 V, undergoing a H1-H2 phase transition without discernible formation of an unstable H3 phase. The results indicate that moderate Mg doping is a facile yet effective strategy to develop high-performance Ni-rich cathode materials.

| S-EPMC6354825 | biostudies-literature

Defective oxygen inert phase stabilized high-voltage nickel-rich cathode for high-energy lithium-ion batteries.

Project description:Pushing layered cathode to higher operating voltage can facilitate the realization of high-energy lithium-ion batteries. However, the released oxygen species initiate materials surface upon highly delithiated states will react severely with electrolyte, accelerating the structure deterioration and triggering the thermal degradation. Here we propose an inert phase of La2Mo2O9 with abundant oxygen vacancies (about 41%) by regulating the annealing temperature to engineer the cathode interface beyond conventional modifications. By employing LiNi0.8Co0.1Mn0.1O2 as a model system and extending to higher voltage-operated LiCoO2 and Li-rich cathode, we demonstrate that the introduced lanthanum and molybdenum ions will transfer electrons to enhance the surface oxygen electronegativities, thus served as "oxygen anchor" to alleviate oxygen evolution. Furthermore, the possible released oxygen can be operando captured and reserved by β-phase La2Mo2O9 depositor for the intrinsic high oxygen vacancy formation energy. The reaction involving oxygen species with electrolyte is fundamentally diminished, thus effectively mitigate the structure deterioration and elevate the electrochemical performances, enabling a 1.5-Ah pouch-type full cell to exhibit negligible 6.0% capacity loss after 400 cycles.

| S-EPMC10700321 | biostudies-literature

Ultrafast fluxional exchange dynamics in electrolyte solvation sheath of lithium ion battery.

Project description:Lithium cation is the charge carrier in lithium-ion battery. Electrolyte solution in lithium-ion battery is usually based on mixed solvents consisting of polar carbonates with different aliphatic chains. Despite various experimental evidences indicating that lithium ion forms a rigid and stable solvation sheath through electrostatic interactions with polar carbonates, both the lithium solvation structure and more importantly fluctuation dynamics and functional role of carbonate solvent molecules have not been fully elucidated yet with femtosecond vibrational spectroscopic methods. Here we investigate the ultrafast carbonate solvent exchange dynamics around lithium ions in electrolyte solutions with coherent two-dimensional infrared spectroscopy and find that the time constants of the formation and dissociation of lithium-ion···carbonate complex in solvation sheaths are on a picosecond timescale. We anticipate that such ultrafast microscopic fluxional processes in lithium-solvent complexes could provide an important clue to understanding macroscopic mobility of lithium cation in lithium-ion battery on a molecular level.

| S-EPMC5344975 | biostudies-literature

A promising bulky anion based lithium borate salt for lithium metal batteries.

Project description:A new salt of lithium trifluoro(perfluoro-tert-butyloxyl)borate (LiTFPFB) which possesses a bulky fluoroalkoxyl functional group in the borate anion has been synthesized for high energy lithium metal batteries. The presence of the bulky fluoroalkoxyl group in the borate anion of LiTFPFB can facilitate ion dissociation and in situ generate a protective film on the Li anode. As a result, LiTFPFB possesses a dramatically improved ionic conductivity and LiFePO4/Li cells using 1.0 M LiTFPFB/PC electrolyte exhibit improved capacity retention especially upon cycling at elevated temperature (60 °C). Ex situ surface analysis reveals that a protective film is formed on the lithium metal anode, which can inhibit further decomposition of the electrolyte. Furthermore, the LiTFPFB based electrolyte also imparts an excellent cycling performance to LiCoO2/Li metal cells for 500 cycles. The outstanding performance of the LiTFPFB salt demonstrates that it is a very promising baseline salt for next generation lithium metal batteries.

| S-EPMC5934741 | biostudies-literature

Stabilizing lithium metal using ionic liquids for long-lived batteries.

Project description:Suppressing dendrite formation at lithium metal anodes during cycling is critical for the implementation of future lithium metal-based battery technology. Here we report that it can be achieved via the facile process of immersing the electrodes in ionic liquid electrolytes for a period of time before battery assembly. This creates a durable and lithium ion-permeable solid-electrolyte interphase that allows safe charge-discharge cycling of commercially applicable Li|electrolyte|LiFePO4 batteries for 1,000 cycles with Coulombic efficiencies >99.5%. The tailored solid-electrolyte interphase is prepared using a variety of electrolytes based on the N-propyl-N-methylpyrrolidinium bis(fluorosulfonyl)imide room temperature ionic liquid containing lithium salts. The formation is both time- and lithium salt-dependant, showing dynamic morphology changes, which when optimized prevent dendrite formation and consumption of electrolyte during cycling. This work illustrates that a simple, effective and industrially applicable lithium metal pretreatment process results in a commercially viable cycle life for a lithium metal battery.

| S-EPMC4909938 | biostudies-literature

A "cation-anion regulation" synergistic anode host for dendrite-free lithium metal batteries.

Project description:Dendritic Li deposition has been "a Gordian knot" for almost half a century, which significantly hinders the practical use of high-energy lithium metal batteries (LMBs). The underlying mechanisms of this dendrite formation are related to the preferential lithium deposition on the tips of the protuberances of the anode surface and also associated with the concentration gradient or even depletion of anions during cycling. Therefore, a synergistic regulation of cations and anions at the interface is vital to promoting dendrite-free Li anodes. An ingenious molecular structure is designed to realize the "cation-anion regulation" with strong interactions between adsorption sites and ions at the molecular level. A quaternized polyethylene terephthalate interlayer with a "lithiophilic" ester building block and an "anionphilic" quaternary ammonium functional block can guide ions to form dendrite-free Li metal deposits at an ultrahigh current density of 10 mA cm-2, enabling stable LMBs.

| S-EPMC5834003 | biostudies-literature

Effects of fluorinated solvents on electrolyte solvation structures and electrode/electrolyte interphases for lithium metal batteries.

Project description:Electrolyte is very critical to the performance of the high-voltage lithium (Li) metal battery (LMB), which is one of the most attractive candidates for the next-generation high-density energy-storage systems. Electrolyte formulation and structure determine the physical properties of the electrolytes and their interfacial chemistries on the electrode surfaces. Localized high-concentration electrolytes (LHCEs) outperform state-of-the-art carbonate electrolytes in many aspects in LMBs due to their unique solvation structures. Types of fluorinated cosolvents used in LHCEs are investigated here in searching for the most suitable diluent for high-concentration electrolytes (HCEs). Nonsolvating solvents (including fluorinated ethers, fluorinated borate, and fluorinated orthoformate) added in HCEs enable the formation of LHCEs with high-concentration solvation structures. However, low-solvating fluorinated carbonate will coordinate with Li+ ions and form a second solvation shell or a pseudo-LHCE which diminishes the benefits of LHCE. In addition, it is evident that the diluent has significant influence on the electrode/electrolyte interphases (EEIs) beyond retaining the high-concentration solvation structures. Diluent molecules surrounding the high-concentration clusters could accelerate or decelerate the anion decomposition through coparticipation of diluent decomposition in the EEI formation. The varied interphase features lead to significantly different battery performance. This study points out the importance of diluents and their synergetic effects with the conductive salt and the solvating solvent in designing LHCEs. These systematic comparisons and fundamental insights into LHCEs using different types of fluorinated solvents can guide further development of advanced electrolytes for high-voltage LMBs.

| S-EPMC7936379 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data