journal article·2025-05-06

Unveiling the Entropic Effect of Electrolytes on Kinetics and Cyclability for Practical Lithium–Sulfur Batteries

Donghyeok Son, Jinuk Kim, Wenhui Zhao, Hannah Cho, Dong Gyu Lee, Junsu Son, Liangliang Xu, Cheol-Young Park, Jungyoon Lee, Ju Hyun Lee, Seungjun Han, Hee-Tak Kim, Tae Kyung Lee, Jinwoo Lee

ACS Nano· Volume 19· Issue 17
Publisher page

Abstract

Lithium–sulfur (Li–S) batteries under low-temperature and lean electrolyte conditions for practical application are hindered by a sluggish conversion reaction, low sulfur utilization, and cycling stability. Herein, we designed a high-entropy (HE) electrolyte by mixing three Li salts. The HE electrolyte simultaneously improves lithium sulfide (Li 2 S) conversion reaction kinetics, sulfur utilization, and cyclability due to the anticlustering effect on lithium polysulfides, three-dimensional Li 2 S growth, and robust anion-derived solid electrolyte interphase layer formation, respectively. Consequently, the HE electrolyte exhibits a high initial reversible capacity (1159.9 mAh g –1 ) and cycling stability for 40 cycles under a low electrolyte-to-sulfur ratio (3.5 μL mg –1 ) at the pouch cell level. In addition, the Li–S cell with HE electrolyte exhibits high cycling stability with a capacity decay of 0.01% per cycle during 200 cycles at −15 °C.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced Battery Technologies Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology, 291 Daehak-Ro, Daejeon 34141, Yuseong-Gu, Republic of Korea

Department of Physics

Ningbo University

Department of Materials Engineering and Convergence Technology, Gyeongsang National University, 501 Jinju-daero, Jinju 52828, Republic of Korea

School of Materials Science and Engineering, Gyeongsang National University, 501 Jinju-daero, Jinju 52828, Republic of Korea

Funding

National Research Foundation of Korea · Korea Forest Service

References (91)

Show source-provided references
1. 10.1016/j.etran.2021.10010310.1016/j.etran.2021.100103 ↗
2. 10.1007/s11814-022-1372-010.1007/s11814-022-1372-0 ↗
3. 10.1016/j.joule.2024.05.01310.1016/j.joule.2024.05.013 ↗
4. 10.3390/batteries909047610.3390/batteries9090476 ↗
5. 10.1038/s41586-021-04139-110.1038/s41586-021-04139-1 ↗
6. 10.1149/2.F10223IF10.1149/2.F10223IF ↗
7. 10.1002/adma.20240063910.1002/adma.202400639 ↗
8. 10.1038/s41467-023-37564-z10.1038/s41467-023-37564-z ↗
9. 10.1002/anie.20221268010.1002/anie.202212680 ↗
10. 10.1021/acsnano.3c0933310.1021/acsnano.3c09333 ↗
11. 10.1021/acsnano.3c1207610.1021/acsnano.3c12076 ↗
12. 10.1016/j.ensm.2023.04.00210.1016/j.ensm.2023.04.002 ↗
13. 10.1002/anie.20231878510.1002/anie.202318785 ↗
14. 10.1039/D1EE03292E10.1039/D1EE03292E ↗
15. 10.1016/j.cej.2023.14147710.1016/j.cej.2023.141477 ↗
16. 10.1021/acsami.2c1090610.1021/acsami.2c10906 ↗
17. 10.1039/D1TA02779D10.1039/D1TA02779D ↗
18. 10.1002/aenm.20230285010.1002/aenm.202302850 ↗
19. 10.1039/C7EE02874A10.1039/C7EE02874A ↗
20. 10.1002/smtd.20190034410.1002/smtd.201900344 ↗
21. 10.1002/adma.20240707010.1002/adma.202407070 ↗
22. 10.1038/s41467-023-44161-710.1038/s41467-023-44161-7 ↗
23. 10.1002/adfm.20220757910.1002/adfm.202207579 ↗
24. 10.1002/anie.20230582810.1002/anie.202305828 ↗
25. 10.1021/jacs.2c1377610.1021/jacs.2c13776 ↗
26. 10.1002/smtd.20190070110.1002/smtd.201900701 ↗
27. 10.1021/acsnano.3c0839510.1021/acsnano.3c08395 ↗
28. 10.1002/adma.20230858710.1002/adma.202308587 ↗
29. 10.1038/s41560-024-01519-510.1038/s41560-024-01519-5 ↗
30. 10.1016/j.cej.2024.15148910.1016/j.cej.2024.151489 ↗
31. 10.1039/D4EE01885K10.1039/D4EE01885K ↗
32. 10.1002/cey2.1010.1002/cey2.10 ↗
33. 10.1021/acsnano.4c0331510.1021/acsnano.4c03315 ↗
34. 10.1002/aenm.20200049310.1002/aenm.202000493 ↗
35. 10.1002/anie.20240633610.1002/anie.202406336 ↗
36. 10.1021/acsenergylett.2c0087410.1021/acsenergylett.2c00874 ↗
37. 10.1002/adma.20227031210.1002/adma.202270312 ↗
38. 10.1016/j.ensm.2023.10304010.1016/j.ensm.2023.103040 ↗
39. 10.1002/ange.20230904610.1002/ange.202309046 ↗
40. 10.1002/adma.20170664310.1002/adma.201706643 ↗
41. 10.1002/inf2.1229110.1002/inf2.12291 ↗
42. 10.1039/D0EE03181J10.1039/D0EE03181J ↗
43. 10.1021/acsnano.4c0303110.1021/acsnano.4c03031 ↗
44. 10.1002/adma.20200502210.1002/adma.202005022 ↗
45. 10.1016/j.joule.2021.06.00910.1016/j.joule.2021.06.009 ↗
46. 10.1002/aenm.20180220710.1002/aenm.201802207 ↗
47. 10.1016/j.jechem.2020.06.05410.1016/j.jechem.2020.06.054 ↗
48. 10.1038/s41560-023-01280-110.1038/s41560-023-01280-1 ↗
49. 10.1021/acsenergylett.4c0135810.1021/acsenergylett.4c01358 ↗
50. 10.1002/adma.20221067710.1002/adma.202210677 ↗
51. 10.1021/acsnano.4c1266010.1021/acsnano.4c12660 ↗
52. 10.1021/acs.jpclett.8b0135910.1021/acs.jpclett.8b01359 ↗
53. 10.1016/j.cej.2022.13663710.1016/j.cej.2022.136637 ↗
54. 10.1149/2.0441805jes10.1149/2.0441805jes ↗
55. 10.1016/j.powera.2024.10015310.1016/j.powera.2024.100153 ↗
56. 10.1021/acs.chemmater.9b0516410.1021/acs.chemmater.9b05164 ↗
57. 10.1002/cssc.20220209510.1002/cssc.202202095 ↗
58. 10.1002/adma.20230737010.1002/adma.202307370 ↗
59. 10.1021/acsomega.8b0302210.1021/acsomega.8b03022 ↗
60. 10.1002/ange.20240157610.1002/ange.202401576 ↗
61. 10.1002/inf2.1204610.1002/inf2.12046 ↗
62. 10.20517/energymater.2021.1710.20517/energymater.2021.17 ↗
63. 10.1007/s43938-024-00045-w10.1007/s43938-024-00045-w ↗
64. 10.1039/D3EE04358D10.1039/D3EE04358D ↗
65. 10.1002/anie.20220346610.1002/anie.202203466 ↗
66. 10.1002/anie.20230546610.1002/anie.202305466 ↗
67. 10.1021/acsami.9b0704810.1021/acsami.9b07048 ↗
68. 10.1038/s41467-018-07975-410.1038/s41467-018-07975-4 ↗
69. 10.1021/ct700301q10.1021/ct700301q ↗
70. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Scalmani, G.; Barone, V.; Petersson, G. A.; Nakatsuji, H.; Li, X.; Caricato, M.; Marenich, A. V.; Bloino, J.; Janesko, B. G.; Gomperts, R.; Mennucci, B.; Hratchian, H. P.; Ortiz, J. V.; Izmaylov, A. F. Gaussian 16, revision A.03; Gaussian, Inc.: Wallingford, CT, 2016.
71. 10.1063/1.338234410.1063/1.3382344 ↗
72. 10.1002/jcc.2175910.1002/jcc.21759 ↗
73. 10.1063/1.46491310.1063/1.464913 ↗
74. 10.1021/jp810292n10.1021/jp810292n ↗
75. Wohlfarth C. · 2008 · 17 · 263
76. Wohlfarth C. · 2015 · 27 · 3710.1007/978-3-662-48168-4_36 ↗
77. 10.1002/jcc.2288510.1002/jcc.22885 ↗
78. 10.1063/1.306016410.1063/1.3060164 ↗
79. 10.1063/1.512139210.1063/1.5121392 ↗
80. 10.1016/j.jpowsour.2017.10.08110.1016/j.jpowsour.2017.10.081 ↗
81. 10.1002/jcc.2122410.1002/jcc.21224 ↗
82. 10.1103/PhysRevLett.45.119610.1103/PhysRevLett.45.1196 ↗
83. 10.1080/08927022.2020.180821510.1080/08927022.2020.1808215 ↗
84. 10.1016/j.nanoen.2020.10491510.1016/j.nanoen.2020.104915 ↗
85. 10.1002/jcc.54005020410.1002/jcc.540050204 ↗
86. 10.1063/1.44811810.1063/1.448118 ↗
87. 10.1063/1.45845210.1063/1.458452 ↗
88. 10.1063/1.131601510.1063/1.1316015 ↗
89. 10.1021/j100096a00110.1021/j100096a001 ↗
90. 10.1103/PhysRevLett.102.07300510.1103/PhysRevLett.102.073005 ↗
91. 10.1039/P2993000079910.1039/P29930000799 ↗