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024 7 _ |a 10.1016/j.jpowsour.2021.229508
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024 7 _ |a 1873-2755
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037 _ _ |a FZJ-2021-05559
082 _ _ |a 620
100 1 _ |a Huang, Chen-Jui
|b 0
245 _ _ |a Origin of shuttle-free sulfurized polyacrylonitrile in lithium-sulfur batteries
260 _ _ |a New York, NY [u.a.]
|c 2021
|b Elsevier
336 7 _ |a article
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520 _ _ |a 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.
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700 1 _ |a Cheng, Ju-Hsiang
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700 1 _ |a Su, Wei-Nien
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700 1 _ |a Partovi-Azar, Pouya
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700 1 _ |a Kuo, Liang-Yin
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700 1 _ |a Tsai, Meng-Che
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700 1 _ |a Lin, Ming-Hsien
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700 1 _ |a Panahian Jand, Sara
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700 1 _ |a Chan, Ting-Shan
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700 1 _ |a Wu, Nae-Lih
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700 1 _ |a Kaghazchi, Payam
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700 1 _ |a Dai, Hongjie
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700 1 _ |a Bieker, Peter Maria
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700 1 _ |a Hwang, Bing-Joe
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773 _ _ |a 10.1016/j.jpowsour.2021.229508
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