skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Operando Studies Reveal Structural Evolution with Electrochemical Cycling in Li–CoS2

Journal Article · · Journal of Physical Chemistry. C
ORCiD logo [1]; ORCiD logo [1];  [2];  [1];  [1];  [1];  [3];  [3]; ORCiD logo [3];  [3];  [3]; ORCiD logo [1]
  1. Univ. of California, Santa Barbara, CA (United States)
  2. Univ. of California, Santa Barbara, CA (United States); Fraunhofer IWM, Freiburg (Germany)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
+ Show Author Affiliations

The desire for high energy density alternatives to Li-ion batteries has led to great interest in energy storage materials not inherently constrained by the capacity limits of standard intercalation electrode materials currently employed in commercial devices. Among the alternatives under consideration are electrode materials with theoretical capacities many times greater than intercalation electrodes, including those that store charge through so-called conversion reactions. However, the vast structural changes that enable the high theoretical capacity of conversion systems contribute to issues of poor efficiency and short cycle life. To better understand the cycling issues in conversion systems, we study the local structure evolution of the cathode active material in LiCoS2 cells. Being metallic, and potentially being capable of redox on both the anion and cation, we would expect CoS2 to be a promising cathode material. Through combined ex situ X-ray absorption near-edge spectroscopy and pair distribution function analysis from operando X-ray total scattering, we describe the reactions that take place over the first 1.5 cycles. In doing so, we identify the irreversible formation of a Co9S8-like local structure with significantly limited electrochemical activity as the primary source of capacity fade. The methods employed here and the insights that emerge inform the rational design of conversion systems for electrochemical energy storage.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1491740
Journal Information:
Journal of Physical Chemistry. C, Vol. 122, Issue 43; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 5 works
Citation information provided by
Web of Science

Figures / Tables (13)

Figure 1(p. 5)figure Figure 1
Figure 2(p. 10)figure Figure 2
Figure 3(p. 12)figure Figure 3
Table 1(p. 14)table Table 1
Figure 4(p. 15)figure Figure 4
Figure 5(p. 16)figure Figure 5
Figure 6(p. 17)figure Figure 6
Figure 7(p. 18)figure Figure 7
Figure 8(p. 19)figure Figure 8
Figure 9(p. 20)figure Figure 9
Figure 10(p. 22)figure Figure 10
Figure 11(p. 23)figure Figure 11
Figure 12(p. 27)figure Figure 12

Similar Records

Tracking the Chemical and Structural Evolution of the TiS2 Electrode in the Lithium-Ion Cell Using Operando X-ray Absorption Spectroscopy
Journal Article · Fri Jun 01 00:00:00 EDT 2018 · Nano Letters · OSTI ID:1491740
+8 more
Local Structure Evolution and Modes of Charge Storage in Secondary Li–FeS 2 Cells
Journal Article · Mon Mar 27 00:00:00 EDT 2017 · Chemistry of Materials · OSTI ID:1491740
+12 more
Nickel-rich Nickel Manganese Cobalt (NMC622) Cathode Lithiation Mechanism and Extended Cycling Effects Using Operando X-ray Absorption Spectroscopy
Journal Article · Fri Dec 11 00:00:00 EST 2020 · Journal of Physical Chemistry. C · OSTI ID:1491740
+6 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY