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Xu GL, Ma T, Sun CJ, et al. Insight into the Capacity Fading Mechanism of Amorphous Se2S5 Confined in Micro/Mesoporous Carbon Matrix in Ether-Based Electrolytes. Nano Lett. 2016;16(4):2663-73doi: 10.1021/acs.nanolett.6b00318.
Xu, G. L., Ma, T., Sun, C. J., Luo, C., Cheng, L., Ren, Y., Heald, S. M., Wang, C., Curtiss, L., Wen, J., Miller, D. J., Li, T., Zuo, X., Petkov, V., Chen, Z., & Amine, K. (2016). Insight into the Capacity Fading Mechanism of Amorphous Se2S5 Confined in Micro/Mesoporous Carbon Matrix in Ether-Based Electrolytes. Nano letters, 16(4), 2663-73. https://doi.org/10.1021/acs.nanolett.6b00318
Xu, Gui-Liang, et al. "Insight into the Capacity Fading Mechanism of Amorphous Se2S5 Confined in Micro/Mesoporous Carbon Matrix in Ether-Based Electrolytes." Nano letters vol. 16,4 (2016): 2663-73. doi: https://doi.org/10.1021/acs.nanolett.6b00318
Xu GL, Ma T, Sun CJ, Luo C, Cheng L, Ren Y, Heald SM, Wang C, Curtiss L, Wen J, Miller DJ, Li T, Zuo X, Petkov V, Chen Z, Amine K. Insight into the Capacity Fading Mechanism of Amorphous Se2S5 Confined in Micro/Mesoporous Carbon Matrix in Ether-Based Electrolytes. Nano Lett. 2016 Apr 13;16(4):2663-73. doi: 10.1021/acs.nanolett.6b00318. Epub 2016 Mar 31. PMID: 27022761.
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Nano Lett. 2016 Apr 13;16(4):2663-73. doi: 10.1021/acs.nanolett.6b00318. Epub 2016 Mar 31.

Insight into the Capacity Fading Mechanism of Amorphous Se2S5 Confined in Micro/Mesoporous Carbon Matrix in Ether-Based Electrolytes.

Nano letters

Gui-Liang Xu, Tianyuan Ma, Cheng-Jun Sun, Chao Luo, Lei Cheng, Yang Ren, Steve M Heald, Chunsheng Wang, Larry Curtiss, Jianguo Wen, Dean J Miller, Tao Li, Xiaobing Zuo, Valeri Petkov, Zonghai Chen, Khalil Amine

Affiliations

  1. Chemical Sciences and Engineering Division, Argonne National Laboratory , Lemont, Illinois 60439, United States.
  2. Materials Science Program, University of Rochester , Rochester, New York 14627, United States.
  3. X-ray Science Division, Argonne National Laboratory , Lemont, Illinois 60439, United States.
  4. Department of Chemical and Biomolecular Engineering, University of Maryland , College Park, Maryland 20742, United States.
  5. Materials Science Division, Argonne National Laboratory , Lemont, Illinois 60439, United States.
  6. Center for Nanoscale Materials, Nanoscience Technology, Argonne National Laboratory , Lemont, Illinois 60439, United States.
  7. Department of Physics, Central Michigan University , Mt. Pleasant, Michigan 48859, United States.

PMID: 27022761 DOI: 10.1021/acs.nanolett.6b00318

Abstract

In contrast to the stable cycle performance of space confined Se-based cathodes for lithium batteries in carbonate-based electrolytes, their common capacity fading in ether-based electrolytes has been paid less attention and not yet well-addressed so far. In this work, the lithiation/delithiation of amorphous Se2S5 confined in micro/mesoporous carbon (Se2S5/MPC) cathode was investigated by in situ X-ray near edge absorption spectroscopy (XANES) and theoretical calculations. The Se2S5/MPC composite was synthesized by a modified vaporization-condensation method to ensure a good encapsulation of Se2S5 into the pores of MPC host. In situ XANES results illustrated that the lithiation/delithiation reversibility of Se component was gradually decreased in ether-based electrolytes, leading to an aggravated formation of long-chain polyselenides during cycling and further capacity decay. Moreover, ab initio calculations revealed that the binding energy of polyselenides (Li2Sen) with carbon host is in an order of Li2Se6 > Li2Se4 > Li2Se. The insights into the failure mechanism of Se-based cathode gain in this work are expected to serve as a guide for future design on high performance Se-based cathodes.

Keywords: Se2S5/MPC cathode; ab initio calculations; batteries; capacity fading; ether-based electrolytes; in situ XANES

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