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@ARTICLE{Huang:903989,
author = {Huang, Chen-Jui and Cheng, Ju-Hsiang and Su, Wei-Nien and
Partovi-Azar, Pouya and Kuo, Liang-Yin and Tsai, Meng-Che
and Lin, Ming-Hsien and Panahian Jand, Sara and Chan,
Ting-Shan and Wu, Nae-Lih and Kaghazchi, Payam and Dai,
Hongjie and Bieker, Peter Maria and Hwang, Bing-Joe},
title = {{O}rigin of shuttle-free sulfurized polyacrylonitrile in
lithium-sulfur batteries},
journal = {Journal of power sources},
volume = {492},
issn = {0378-7753},
address = {New York, NY [u.a.]},
publisher = {Elsevier},
reportid = {FZJ-2021-05559},
pages = {229508 -},
year = {2021},
note = {Kein Post-print vorhanden.},
abstract = {Sulfurized polyacrylonitrile (S-cPAN) shows an intrinsic
shuttle-free capability during cycling with high reversible
capacity, making it a promising material for lithium-sulfur
(Li–S) battery. However, the lithiation/delithiation
mechanism of S-cPAN is still debatable and unclear. In this
work, the fundamental reaction mechanism of S-cPAN cathode
material is unveiled by in-situ Raman and in-situ X-ray
absorption (XAS) spectroscopies. Together with density
functional theory calculation, the formation of -N-Sx-N- (x
< 4) bridges besides C–S- and –S-S- bonds during the
synthesis process is proposed. These sulfur-nitrogen bonds
and their strong interactions in the S-cPAN compounds are
first observed to account for the proposed solid-solid
transformation during the lithiation/delithiation of S-cPAN.
Surprisingly, the cPAN backbone is also found to be involved
in the charge compensation while the ordered Li2S along the
nitrogen edge on the PAN matrix is suggested to form when
S-cPAN is fully lithiated. The proposed modified mechanism
deciphers the outstanding electrochemical performance of
S-cPAN, providing a new pathway for designing high capacity,
shuttle-free cathode materials for next-generation Li–S
batteries, and a new perspective of sulfur chemistry.},
cin = {IEK-1},
ddc = {620},
cid = {I:(DE-Juel1)IEK-1-20101013},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000635068900002},
doi = {10.1016/j.jpowsour.2021.229508},
url = {https://juser.fz-juelich.de/record/903989},
}