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Simultaneous Monitoring of Crystalline Active Materials and Resistance Evolution in Lithium-Sulfur Batteries

submitted on 24.10.2019, 13:37 and posted on 28.10.2019, 21:09 by Yu-Chuan Chien, Ashok Menon, William Brant, Daniel Brandell, Matthew Lacey
Operando X-ray diffraction (XRD) is a valuable tool for studying secondary battery materials as it allows for the direct correlation of electrochemical behavior with structural changes of crystalline active materials. This is especially true for the lithium-sulfur chemistry, in which energy storage capability depends on the complex growth and dissolution kinetics of lithium sulfide (Li2S) and sulfur (S8) during discharge and charge, respectively. In this work, we present a novel development of this method through combining operando XRD with simultaneous and continuous resistance measurement using an Intermittent Current Interruption (ICI) method. We show that a coefficient of diffusion resistance, which reflects the transport properties in the sulfur/carbon composite electrode, can be determined from analysis of each current interruption. Its relationship to the established Warburg impedance model is validated theoretically and experimentally. We also demonstrate for an optimized electrode formulation and cell construction that the diffusion resistance increases sharply at the discharge end point, which is consistent with the blocking of pores in the carbon host matrix. The combination of XRD with ICI allows for a direct correlation of structural changes with not only electrochemical properties but also energy loss processes at a non-equilibrium state, and therefore is a valuable technique for the study of a wide range of energy storage chemistries.


Swedish Energy Agency: Sulfur Technology Advanced Research Concept (42762-1)

Swedish Energy Agency: Functional materials for future high-energy Li-S batteries (42031-1)

Swedish Foundation for Strategic Research: Swedish national graduate school in neutron scattering (SwedNess)


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Uppsala University



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Declaration of Conflict of Interest

The authors declare no conflict of interest.