Understanding the Origin of Irreversible Capacity loss in Non-Carbonized Carbonate - based Metal Organic Framework (MOF) Sulfur hosts for Lithium - Sulfur battery

Shanthi, Pavithra M.; Hanumantha, Prashanth J.; Gattu, Bharat; Sweeney, Matthew; Datta, Moni K.; Kumta, Prashant N.

doi:10.1016/j.electacta.2017.01.115

Understanding the Origin of Irreversible Capacity loss in Non-Carbonized Carbonate - based Metal Organic Framework (MOF) Sulfur hosts for Lithium - Sulfur battery

Journal Article · Fri Jan 20 00:00:00 EST 2017 · Electrochimica Acta

DOI:https://doi.org/10.1016/j.electacta.2017.01.115· OSTI ID:1429050

Shanthi, Pavithra M. ^[1]; Hanumantha, Prashanth J. ^[2]; Gattu, Bharat ^[3]; Sweeney, Matthew ^[4]; Datta, Moni K. ^[2]; Kumta, Prashant N. ^[5]

Univ. of Pittsburgh, PA (United States). Dept. of Chemical and Petroleum Engineering; University of Pittsburgh
Univ. of Pittsburgh, PA (United States). Dept. of Bioengineering
Univ. of Pittsburgh, PA (United States). Dept. of Chemical and Petroleum Engineering
Univ. of Maryland Baltimore County (UMBC), Baltimore, MD (United States). Dept. of Chemical Engineering
Univ. of Pittsburgh, PA (United States). Dept. of Chemical and Petroleum Engineering. Dept. of Bioengineering. Dept. of Mechanical Engineering and Materials Science. Center for Complex Engineered Multifunctional Materials

Li-Sulfur (Li-S) batteries are emergent next-generation energy storage devices due to their very high specific energy density (~2567 Wh g^-1) but are limited by polysulfide dissolution issues. In this paper, chemically synthesized sulfur containing non-carbonized metal organic framework (S-MOF) cathodes show initial specific capacities of 1476 mAh g^-1 stabilizing at ~609 mAh g^-1 with almost no fade for over 200 cycles. Post-cycled separators of the S – MOF cathodes display complete absence of polysulfides after cycle 1, 20 and 200, respectively. It was identified that the occurrence of carbonate species in the MOF structure resulted in the formation of C-S bonded species causing retention of polysulfide at the electrode surface ensuring long-term stability. However, this observed capacity drop during the first 10 cycles is attributed to the oxidation of some of the infiltrated sulfur by the MOF as determined by electrochemical and X-ray photoelectron spectroscopy (XPS) analyses. Nevertheless, the negligible fade rate (0.0014% cycle^-1) and complete prevention of polysulfide dissolution renders these cathodes most promising candidates for Li-S batteries. Finally, understanding of this transformation behavior in sulfur-containing MOF is essential to engineer chemically-bonded host-structures capable of efficient polysulfide trapping, a key pathway to establishing novel platforms for achieving high power Li – S batteries.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Pittsburgh, PA (United States)

Sponsoring Organization:: National Science Foundation (NSF) (United States); USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: EE0006825

OSTI ID:: 1429050

Alternate ID(s):: OSTI ID: 1417083
OSTI ID: 22656937

Journal Information:: Electrochimica Acta, Journal Name: Electrochimica Acta Vol. 229; ISSN 0013-4686

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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