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Atomistic View of Evolution and Reactivity of Polysulfide Redox Species in Li-S Batteries


EMSL Project ID
48846

Abstract

The Joint Center for Energy Storage Research (JCESR) is performing transformational research to overcome critical scientific and technical barriers in achieving ‘beyond Li-Ion battery technology’. Li-Sulfur redox chemistry is one of the promising candidates, which could provide cost effective and high performing energy storage devices for both mobile and stationary applications. The major scientific barriers in achieving reliable Li-Sulfur battery technology is the knowledge gap in our understanding about the evolution and reactivity of polysulfide redox species during electrochemical process. In particular, the reduction of the elemental sulfur cathode leads to varying types of polysulfides, each with unique reactivity towards electrolytes and the lithium anode, which adversely affects the longevity of the battery. The JCSER team plans on achieving breakthroughs across these key scientific barriers using unique multi-modal in situ spectroscopies to correlate the evolution and reactivity of polysulfide redox species with their functional performance. The results will be used to establish a close feedback loop between collaborators, starting with in situ NMR, EPR & TEM spectroscopies at EMSL, on to synchrotron in situ X-ray analysis at ALS along with complimentary theoretical analysis, to identification of optimal materials and the testing of these materials in realistic devices, and back to in situ spectroscopic analysis of the devices. In-situ experimental methods that will be developed and exploited in this work, such as in-situ NMR and TEM, will also be applicable to research in the field of materials for energy storage/conversion devices and therefore a wide range of the EMSL user community will benefit from these efforts.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2015-10-01
End Date
2017-09-30
Status
Closed

Team

Principal Investigator

Karl Mueller
Institution
Pacific Northwest National Laboratory

Co-Investigator(s)

Nigel Browning
Institution
University of Liverpool

Team Members

Abraham Martinez
Institution
Pacific Northwest National Laboratory

Carolyn Sturges
Institution
Richland School District

Alexander Krol
Institution
Washington & Jefferson College

Cynthia Ly
Institution
California Polytechnic State University

Eric Jensen
Institution
Pacific Northwest National Laboratory

Wesley Henderson
Institution
Pacific Northwest National Laboratory

Robbie Iuliucci
Institution
Washington & Jefferson College

Jie Xiao
Institution
University of Arkansas, Fayetteville

Vijayakumar Murugesan
Institution
Pacific Northwest National Laboratory

Niranjan Govind
Institution
Pacific Northwest National Laboratory

Jun Liu
Institution
Yale University

Related Publications

Nandasiri MI, LE Camacho-Forero, AM Schwarz, V Shutthanandan, S Thevuthasan, PB Balbuena, KT Mueller, and V Murugesan. 2017. "In-situ chemical imaging of Solid-Electrolyte Interphase layer evolution in Li-S batteries." Chemistry of Materials 29(11):4728–4737. doi:10.1021/acs.chemmater.7b00374
Shutthanandan V., M.I. Nandasiri, J. Zheng, M.H. Engelhard, W. Xu, S. Thevuthasan, and V. Murugesan. 2019. "Applications of XPS in the Characterization of Battery Materials." Journal of Electron Spectroscopy and Related Phenomena 231. PNNL-SA-134570. doi:10.1016/j.elspec.2018.05.005