TY  - JOUR
AU  - Huang, Chen-Jui
AU  - Cheng, Ju-Hsiang
AU  - Su, Wei-Nien
AU  - Partovi-Azar, Pouya
AU  - Kuo, Liang-Yin
AU  - Tsai, Meng-Che
AU  - Lin, Ming-Hsien
AU  - Panahian Jand, Sara
AU  - Chan, Ting-Shan
AU  - Wu, Nae-Lih
AU  - Kaghazchi, Payam
AU  - Dai, Hongjie
AU  - Bieker, Peter Maria
AU  - Hwang, Bing-Joe
TI  - Origin of shuttle-free sulfurized polyacrylonitrile in lithium-sulfur batteries
JO  - Journal of power sources
VL  - 492
SN  - 0378-7753
CY  - New York, NY [u.a.]
PB  - Elsevier
M1  - FZJ-2021-05559
SP  - 229508 -
PY  - 2021
N1  - Kein Post-print vorhanden.
AB  - 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.
LB  - PUB:(DE-HGF)16
UR  - <Go to ISI:>//WOS:000635068900002
DO  - DOI:10.1016/j.jpowsour.2021.229508
UR  - https://juser.fz-juelich.de/record/903989
ER  -