Reductive reactions via excess Li in mixture electrolytes of Li ion batteries: an ab initio molecular dynamics study

Literature Information

Publication Date 2019-02-12
DOI 10.1039/C8CP04907F
Impact Factor 3.676
Authors

Woon Ih Choi, Min Sik Park, Youngseon Shim, Dong Young Kim, Yoon-Sok Kang, Hyo Sug Lee, Meiten Koh


View Original

Abstract

The electro-reduction of battery electrolytes plays a critical role in the formation of solid–electrolyte interphase (SEI) layers on the surfaces of negative electrodes. These layers have a significant influence on the performance of rechargeable battery cells. Using ab initio molecular dynamics, we demonstrate the electro-reduction of mixture electrolytes computationally by adding a certain number of excess Li+ first to form the solvation structure and the same number of electrons later for reductive reactions. Our method enables direct observations of the ring opening of one cyclic carbonate followed by merging with another solvent molecule as well as gas generation. When we examined FEC- and EC-based electrolytes, we were able to observe the differences in terms of reaction products. In particular, the two gaseous products that are generated the most are in accordance with recent in situ gas measurements in the literature. The different reaction products of each electrolyte also match well with the SEI constituents reported experimentally. By tracing reaction pathways, we found that Li+ ions facilitate many otherwise difficult electrochemical reactions, presumably by lowering energy barriers. We also found that the excess Li+ forms cationic clusters of Li2PF6+, which enable the reductive decomposition of salt anions and which do not occur easily simply by increasing the electronic occupation. Based on the reaction products of FEC-based electrolytes, here we propose a possible mechanism of polymerization through aldehyde intermediates that are known to bond with surrounding radical anions.

Related Literature

The first ternary tin(ii) nitride: NaSnN

Nicholas S. P. Watney, Zoltán A. Gál, Matthew D. S. Webster, Simon J. Clarke

2005-07-20 Communication

DOI: 10.1039/B505208D

Ru(iv)-catalyzed isomerization of allylamines in water: A highly efficient procedure for the deprotection of N-allylic amines

Victorio Cadierno, Sergio E. García-Garrido, José Gimeno, Noel Nebra

2005-07-13 Communication

DOI: 10.1039/B506788J

A simple synthesis of mesoporous carbons with tunable mesopores using a colloidal template-mediated vapor deposition polymerization

Jyongsik Jang, Byungkwon Lim, Moonjung Choi

2005-07-22 Communication

DOI: 10.1039/B506265A

In situ formation of ligandandcatalyst—application in ruthenium-catalyzed enantioselective reduction of ketones

Patrik Västilä, Jenny Wettergren, Hans Adolfsson

2005-07-12 Communication

DOI: 10.1039/B505516D

The vicinal F–C–C–F moiety as a tool for influencing peptide conformation

Martin Schüler, David O'Hagan, Alexandra M. Z. Slawin

2005-07-14 Communication

DOI: 10.1039/B506010A

Precise synthesis of poly(macromonomer)s containing sugars by repetitive ring-opening metathesis polymerisation

James J. Murphy, Kotohiro Nomura

2005-07-13 Communication

DOI: 10.1039/B506877K

Inside front cover

Cover

DOI: 10.1039/B511384A

Simple iron-aminecatalysts for the cross-coupling of aryl Grignards with alkyl halides bearing β-hydrogens

Robin B. Bedford, Duncan W. Bruce, Robert M. Frost, Michael Hird

2005-07-22 Communication

DOI: 10.1039/B507133J

Simple and quick chemical aminoacylation of tRNA in cationic micellar solution under ultrasonic agitation

Naoto Hashimoto, Keiko Ninomiya, Takamasa Endo, Masahiko Sisido

2005-08-09 Communication

DOI: 10.1039/B508194G

You might also like

Compound Q&A

How should waste containing N-Methoxy-N-methyl-1,3-thiazole-5-carboxamide (CAS: 898825-89-3) be handled?

Waste containing N-Methoxy-N-methyl-1,3-thiazole-5-carboxamide (CAS: 898825-89-3...

898825-89-3N-Methoxy-N-methyl-1...
Compound Q&A

How should N-(4-Biphenylyl)dibenzo[b,d]furan-4-amine (CAS: 1318338-47-4) be stored?

N-(4-Biphenylyl)dibenzo[b,d]furan-4-amine should be stored in a tightly sealed c...

1318338-47-4N-(4-Biphenylyl)dibe...
Compound Q&A

What is the market or research trend for 3-Acetamido-5-amino-2,4,6-triiodobenzoic acid (CAS: 1713-07-1)?

The market for 3-Acetamido-5-amino-2,4,6-triiodobenzoic acid (CAS: 1713-07-1) is...

1713-07-13-Acetamido-5-amino-...
Compound Q&A

How should Benzyl 2-O-acetyl-3,4,6-tri-O-benzyl-beta-D-galactopyranoside (CAS: 61820-03-9) be stored?

Benzyl 2-O-acetyl-3,4,6-tri-O-benzyl-beta-D-galactopyranoside (CAS: 61820-03-9) ...

61820-03-9Benzyl 2-O-acetyl-3,...
Compound Q&A

What regulatory guidelines apply to 2-Ethylpiperazine dihydrochloride (CAS: 438050-52-3)?

2-Ethylpiperazine dihydrochloride (CAS: 438050-52-3) is regulated under the Glob...

438050-52-32-Ethylpiperazine di...
Compound Q&A

What regulatory guidelines apply to 1,1'-[1,3-Phenylenebis(methylene)]bis(3-methyl-1H-pyrrole-2,5-dione) (CAS: 119462-56-5)?

1,1'-[1,3-Phenylenebis(methylene)]bis(3-methyl-1H-pyrrole-2,5-dione) (CAS: 11946...

119462-56-51,1'-[1,3-Phenyleneb...
Compound Q&A

Are there alternatives to 5-Fluoro-2-(1-pyrrolidinyl)pyridine (CAS: 1287217-79-1) in synthesis?

Several alternatives can be used in the synthesis of 5-Fluoro-2-(1-pyrrolidinyl)...

1287217-79-15-Fluoro-2-(1-pyrrol...
Compound Q&A

What precautions should be taken when handling 6-Bromoimidazo[1,2-a]pyridin-8-amine (CAS: 676371-00-9)?

When handling 6-Bromoimidazo[1,2-a]pyridin-8-amine, it is important to wear appr...

676371-00-96-Bromoimidazo[1,2-a...
Compound Q&A

Are there alternatives to (2S,4R)-4-(4-Nitrobenzyl)pyrrolidine-2-carboxylic acid hydrochloride (CAS: 1049740-22-8) in synthesis?

Alternatives to (2S,4R)-4-(4-Nitrobenzyl)pyrrolidine-2-carboxylic acid hydrochlo...

1049740-22-8(2S,4R)-4-(4-Nitrobe...

Source Journal

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
Articles per Year: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

Recommended Compounds

Recommended Suppliers

Disclaimer
This page provides academic journal information for reference and research purposes only. We are not affiliated with any journal publishers and do not handle publication submissions. For publication-related inquiries, please contact the respective journal publishers directly.
If you notice any inaccuracies in the information displayed, please contact us at support@chemtradehub.com. We will promptly review and address your concerns.