Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 114, Issue 5, Pages 840-845Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1615837114
Keywords
lithium-sulfur batteries; catalytic oxidation; metal sulfides; graphene; polysulfide adsorption
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Funding
- Assistant Secretary for Energy Efficiency and Renewable Energy
- Office of Vehicle Technologies
- Battery Materials Research Program of the US Department of Energy
- National Natural Science Foundation of China [11404017]
- Technology Foundation for Selected Overseas Chinese Scholar
- Ministry of Human Resources and Social Security of China
- program for New Century Excellent Talents in University [NCET-12-0033]
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Polysulfide binding and trapping to prevent dissolution into the electrolyte by a variety of materials has been well studied in Li-S batteries. Here we discover that some of those materials can play an important role as an activation catalyst to facilitate oxidation of the discharge product, Li2S, back to the charge product, sulfur. Combining theoretical calculations and experimental design, we select a series of metal sulfides as a model system to identify the key parameters in determining the energy barrier for Li2S oxidation and polysulfide adsorption. We demonstrate that the Li2S decomposition energy barrier is associated with the binding between isolated Li ions and the sulfur in sulfides; this is the main reason that sulfide materials can induce lower overpotential compared with commonly used carbon materials. Fundamental understanding of this reaction process is a crucial step toward rational design and screening of materials to achieve high reversible capacity and long cycle life in Li-S batteries.
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