%0 Journal Article
%A Huang, Chen-Jui
%A Cheng, Ju-Hsiang
%A Su, Wei-Nien
%A Partovi-Azar, Pouya
%A Kuo, Liang-Yin
%A Tsai, Meng-Che
%A Lin, Ming-Hsien
%A Panahian Jand, Sara
%A Chan, Ting-Shan
%A Wu, Nae-Lih
%A Kaghazchi, Payam
%A Dai, Hongjie
%A Bieker, Peter Maria
%A Hwang, Bing-Joe
%T Origin of shuttle-free sulfurized polyacrylonitrile in lithium-sulfur batteries
%J Journal of power sources
%V 492
%@ 0378-7753
%C New York, NY [u.a.]
%I Elsevier
%M FZJ-2021-05559
%P 229508 -
%D 2021
%Z Kein Post-print vorhanden.
%X 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.
%F PUB:(DE-HGF)16
%9 Journal Article
%U <Go to ISI:>//WOS:000635068900002
%R 10.1016/j.jpowsour.2021.229508
%U https://juser.fz-juelich.de/record/903989