A chemically stabilized sulfur cathode for lean electrolyte lithium sulfur batteries.

carbon chemical bonding lean electrolyte lithium sulfur batteries oxygen

Journal

Proceedings of the National Academy of Sciences of the United States of America
ISSN: 1091-6490
Titre abrégé: Proc Natl Acad Sci U S A
Pays: United States
ID NLM: 7505876

Informations de publication

Date de publication:
30 06 2020
Historique:
pubmed: 20 6 2020
medline: 20 6 2020
entrez: 20 6 2020
Statut: ppublish

Résumé

Lithium sulfur batteries (LSBs) are promising next-generation rechargeable batteries due to the high gravimetric energy, low cost, abundance, nontoxicity, and high sustainability of sulfur. However, the dissolution of high-order polysulfide in electrolytes and low Coulombic efficiency of Li anode require excess electrolytes and Li metal, which significantly reduce the energy density of LSBs. Quasi-solid-state LSBs, where sulfur is encapsulated in the micropores of carbon matrix and sealed by solid electrolyte interphase, can operate under lean electrolyte conditions, but a low sulfur loading in carbon matrix (<40 wt %) and low sulfur unitization (<70%) still limit the energy density in a cell level. Here, we significantly increase the sulfur loading in carbon to 60 wt % and sulfur utilization to ∼87% by dispersing sulfur in an oxygen-rich dense carbon host at a molecular level through strong chemical interactions of C-S and O-S. In an all-fluorinated organic lean electrolyte, the C/S cathode experiences a solid-state lithiation/delithiation reaction after the formation of solid electrolyte interphase in the first deep lithiation, completely avoiding the shuttle reaction. The chemically stabilized C/S composite retains a high reversible capacity of 541 mAh⋅g

Identifiants

pubmed: 32554498
pii: 2006301117
doi: 10.1073/pnas.2006301117
pmc: PMC7334495
doi:

Types de publication

Journal Article Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, Non-P.H.S.

Langues

eng

Sous-ensembles de citation

IM

Pagination

14712-14720

Déclaration de conflit d'intérêts

The authors declare no competing interest.

Références

Nat Commun. 2013;4:1481
pubmed: 23403582
Angew Chem Int Ed Engl. 2012 Apr 10;51(15):3591-5
pubmed: 22383067
Adv Mater. 2011 Dec 15;23(47):5641-4
pubmed: 22052740
Acc Chem Res. 2013 May 21;46(5):1125-34
pubmed: 23095063
Nano Lett. 2014 Jun 11;14(6):3550-5
pubmed: 24844948
Angew Chem Int Ed Engl. 2015 Mar 27;54(14):4325-9
pubmed: 25663183
Nat Mater. 2009 Apr;8(4):320-4
pubmed: 19305398
Adv Mater. 2014 Aug 13;26(30):5113-8
pubmed: 24897930
Chem Rev. 2018 Dec 12;118(23):11433-11456
pubmed: 30500179
J Am Chem Soc. 2012 Nov 14;134(45):18510-3
pubmed: 23101502
Nano Lett. 2011 Oct 12;11(10):4288-94
pubmed: 21928817
Nat Mater. 2009 Jun;8(6):500-6
pubmed: 19448613
Nano Lett. 2011 Jul 13;11(7):2644-7
pubmed: 21699259
Nat Chem. 2015 Jan;7(1):19-29
pubmed: 25515886
Nat Commun. 2014 Mar 03;5:3410
pubmed: 24583928
Sci Rep. 2014 Apr 29;4:4842
pubmed: 24776750
J Am Chem Soc. 2015 Sep 23;137(37):12143-52
pubmed: 26325146
Nat Mater. 2016 Dec 20;16(1):45-56
pubmed: 27994251
Nat Commun. 2011;2:325
pubmed: 21610728
J Am Chem Soc. 2014 Mar 26;136(12):4659-63
pubmed: 24580375
J Am Chem Soc. 2011 Nov 23;133(46):18522-5
pubmed: 22017295
J Am Chem Soc. 2013 Jan 16;135(2):763-7
pubmed: 23234561
Nat Commun. 2013;4:1331
pubmed: 23299881
Adv Mater. 2018 May;30(21):e1706102
pubmed: 29575163
Nature. 2009 Mar 12;458(7235):190-3
pubmed: 19279634
Nat Nanotechnol. 2018 Aug;13(8):715-722
pubmed: 30013215
Nat Mater. 2013 Jun;12(6):518-22
pubmed: 23584143
Sci Rep. 2012;2:698
pubmed: 23019519
Nano Lett. 2017 May 10;17(5):3061-3067
pubmed: 28448154
Nat Mater. 2019 May;18(5):496-502
pubmed: 30886397
Nat Mater. 2011 Dec 15;11(1):19-29
pubmed: 22169914
Angew Chem Int Ed Engl. 2011 Jun 20;50(26):5904-8
pubmed: 21591036

Auteurs

Chao Luo (C)

Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD 20742.
Department of Chemistry and Biochemistry, George Mason University, Fairfax, VA 22030.

Enyuan Hu (E)

Chemistry Division, Brookhaven National Laboratory, Upton, NY 11973.

Karen J Gaskell (KJ)

Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742.

Xiulin Fan (X)

Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD 20742.

Tao Gao (T)

Department of Chemical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139.

Chunyu Cui (C)

Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD 20742.

Sanjit Ghose (S)

National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY 11973.

Xiao-Qing Yang (XQ)

Chemistry Division, Brookhaven National Laboratory, Upton, NY 11973.

Chunsheng Wang (C)

Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD 20742; cswang@umd.edu.
Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742.

Classifications MeSH