Formation of Multilayer Graphene Domains with Strong Sulfur-Carbon Interaction and Enhanced Sulfur Reduction Zones for Lithium-Sulfur Battery Cathodes

Perez?Beltran, Saul; Balbuena, Perla B.

doi:10.1002/cssc.201702446

Title: Formation of Multilayer Graphene Domains with Strong Sulfur-Carbon Interaction and Enhanced Sulfur Reduction Zones for Lithium-Sulfur Battery Cathodes

Journal Article · Mon Feb 12 00:00:00 EST 2018 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.201702446· OSTI ID:1460744

Perez?Beltran, Saul ^[1];

^[1]

Texas A & M Univ., College Station, TX (United States). Dept. of Chemical Engineering

Abstract A newly designed sulfur/graphene computational model emulates the electrochemical behavior of a Li–S battery cathode, promoting the S–C interaction through the edges of graphene sheets. A random mixture of eight‐membered sulfur rings mixed with small graphene sheets is simulated at 64 wt %sulfur loading. Structural stabilization and sulfur reduction calculations are performed with classical reactive molecular dynamics. This methodology allowed the collective behavior of the sulfur and graphene structures to be accounted for. The sulfur encapsulation induces ring opening and the sulfur phase evolves into a distribution of small chain‐like structures interacting with C through the graphene edges. This new arrangement of the sulfur phase not only leads to a less pronounced volume expansion during sulfur reduction but also to a different discharge voltage profile, in qualitative agreement with earlier reports on sulfur encapsulation in microporous carbon structures. The Li ₂ S phase grows around ensembles of parallel graphene nanosheets during sulfur reduction. No diffusion of sulfur or lithium between graphene nanosheets is observed, and extended Li ₂ S domains bridging the space between carbon ensembles are suppressed. The results emphasize the importance of morphology on the electrochemical performance of the composite material. The sulfur/graphene model outlined here provides new understanding of the graphene effects on the sulfur reduction behavior and the role that van der Waals interactions may play in promoting formation of multilayer graphene ensembles and small Li ₂ S domains during sulfur reduction.

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Research Organization:: Texas A & M Univ., College Station, TX (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE

Contributing Organization:: Texas A&M High Performance Computing Center; Texas Advanced Computing Center

Grant/Contract Number:: EE0008210; EE0006832

OSTI ID:: 1460744

Alternate ID(s):: OSTI ID: 1426313

Journal Information:: ChemSusChem, Vol. 11, Issue 12; ISSN 1864-5631

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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