In situ TEM observation of electrochemical lithiation of sulfur confined within inner cylindrical pores of carbon nanotubes

Kim, Hyea; Lee, Jung Tae; Magasinski, Alexandre; Zhao, Kejie; Liu, Yang; Yushin, Gleb

doi:10.1002/aenm.201501306

In situ TEM observation of electrochemical lithiation of sulfur confined within inner cylindrical pores of carbon nanotubes

Journal Article · Mon Oct 26 00:00:00 EDT 2015 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.201501306· OSTI ID:1238588

Kim, Hyea ^[1]; Lee, Jung Tae ^[2]; Magasinski, Alexandre ^[2]; Zhao, Kejie ^[3]; Liu, Yang ^[4]; Yushin, Gleb ^[2]

Georgia Inst. of Technology, Atlanta, GA (United States); Sila Nanotechnologies, Inc., Alameda CA (United States)
Georgia Inst. of Technology, Atlanta, GA (United States)
Purdue University, West Lafayette IN (United States)
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Lithium insertion into sulfur confined within 200 nm cylindrical inner pores of individual carbon nanotubes (CNTs) was monitored in-situ in a transmission electron microscope (TEM). This electrochemical reaction was initiated at one end of the S-filled CNTs. The material expansion during lithiation was accommodated by the expansion into the remaining empty pore volume and no fracture of the CNT walls was detected. A sharp interface between the initial and lithiated S was observed. The reaction front was flat, oriented perpendicular to the confined S cylinder and propagated along the cylinder length. Lithiation of S in the proximity of conductive carbon proceeded at the same rate as the one in the center of the pore, suggesting the presence of electron pathways at the Li₂S/S interface. Density of states (DOS) calculations further confirmed this hypothesis. In-situ electron diffraction showed a direct phase transformation of S into nanocrystalline Li₂S without detectable formation of any intermediates, such as polysulfides and LiS. These important insights may elucidate some of the reaction mechanisms and guide the improvements in the design of C-S nanocomposites for high specific energy Li-S batteries. As a result, the proposed use of conductive CNTs with tunable pore diameter as cylindrical reaction vessels for in-situ TEM studies of electrochemical reactions proved to be highly advantageous and may help to resolve the on-going problems in battery technology.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC04-94AL85000

OSTI ID:: 1238588

Report Number(s):: SAND--2015--6324J; 606209

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 24 Vol. 5; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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