title: Following the transient reactions in lithium-sulfur batteries using an in situ nuclear magnetic resonance technique.
abstract: A fundamental understanding of electrochemical reaction pathways is critical to improving the performance of Li-S batteries, but few techniques can be used to directly identify and quantify the reaction species during disharge/charge cycling processes in real time. Here, an in situ (7)Li NMR technique employing a specially designed cylindrical microbattery was used to probe the transient electrochemical and chemical reactions occurring during the cycling of a Li-S system. In situ NMR provides real time, semiquantitative information related to the temporal evolution of lithium polysulfide allotropes during both discharge/charge processes. This technique uniquely reveals that the polysulfide redox reactions involve charged free radicals as intermediate species that are difficult to detect in ex situ NMR studies. Additionally, it also uncovers vital information about the (7)Li chemical environments during the electrochemical and parasitic reactions on the Li metal anode. These new molecular-level insights about transient species and the associated anode failure mechanism are crucial to delineating effective strategies to accelerate the development of Li-S battery technologies.
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Jie
authors.initials: J
authors.lastname: Xiao
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Jian Zhi
authors.initials: JZ
authors.lastname: Hu
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Honghao
authors.initials: H
authors.lastname: Chen
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: M
authors.initials: M
authors.lastname: Vijayakumar
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Jianming
authors.initials: J
authors.lastname: Zheng
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Huilin
authors.initials: H
authors.lastname: Pan
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Eric D
authors.initials: ED
authors.lastname: Walter
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Mary
authors.initials: M
authors.lastname: Hu
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Xuchu
authors.initials: X
authors.lastname: Deng
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Ju
authors.initials: J
authors.lastname: Feng
authors.affiliation: ‡Electrochemical Power Systems Laboratory, Hawaii Natural Energy Institute, School of Ocean and Earth Science and Technology, University of Hawaii-Manoa, Honolulu, Hawaii 96822, United States.
authors.forename: Bor Yann
authors.initials: BY
authors.lastname: Liaw
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Meng
authors.initials: M
authors.lastname: Gu
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Zhiqun Daniel
authors.initials: ZD
authors.lastname: Deng
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Dongping
authors.initials: D
authors.lastname: Lu
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Suochang
authors.initials: S
authors.lastname: Xu
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Chongmin
authors.initials: C
authors.lastname: Wang
authors.affiliation: †Joint Center for Energy Storage Research, Pacific Northwest National Laboratory, Richland, Washington 99352, United States.
authors.forename: Jun
authors.initials: J
authors.lastname: Liu
keywords: Li−S batteries; energy storage; in situ NMR; radicals