journal article·2024-10-08Open access

Oxygen-Incorporated Lithium-Rich Iron Sulfide Cathodes for Li-Ion Batteries with Boosted Material Stability and Electrochemical Performance

Adane G. Hailemariam, Zeru Syum, Tadios T. Mamo, Mohammad Qorbani, Cheng-Rong Hsing, Amr Sabbah, Shaham Quadir, Khasim S. Bayikadi, Heng-Liang Wu, Ching-Ming Wei, Li-Chyong Chen, Kuei-Hsien Chen

Chemistry of Materials· Volume 36· Issue 19

Abstract

High Resolution Image Download MS PowerPoint Slide Affordable and environmentally friendly electrode materials with multielectron redox reactions are imperative for the advancement of next-generation Li-ion batteries. In this context, the Li-rich layered iron sulfide cathode material (i.e., Li 2 FeS 2 ) stands out as a promising candidate due to its unique multielectron cationic and anionic redox features. However, its practical application is hampered by inherent limitations in terms of poor structural stability and cycling performance. Herein, we conduct a systematic investigation into the impact of anionic substitution, where sulfur is partially replaced with oxygen, on the structural stability, intrinsic conductivity, and electrochemical properties of the Li 2 FeS 2 cathode. First-principle calculations confirm that an optimum amount of oxygen incorporation is beneficial to stabilize the crystal structure and improve Li ion diffusion. Furthermore, cathodes with oxygen incorporation exhibit significant structural stability even when exposed to air for 24 h, demonstrating resistance against moisture. The Li 2 FeS 1.8 O 0.2 cathode achieves a higher Coulombic efficiency of ∼100%, charge–discharge capacity of 310 mA h g –1 after 100 cycles, and a remarkable capacity recovery of around 94% following rate capability tests spanning 75 cycles. These findings introduce an innovative anion substitution approach for the development of Li-rich layered sulfide cathode materials, effectively mitigating structural deterioration.
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Research context

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

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Affiliations

Institute of Atomic and Molecular Sciences, Academia Sinica, Taipei 10617, Taiwan

Sustainable Chemical Science and Technology, Taiwan International Graduate Program, Academia Sinica, Nangang, Taipei 11529, Taiwan

Institute of Chemistry, Academia Sinica, Nangang, Taipei 11529, Taiwan

Department of Applied Chemistry, National Yang-Ming Chiao Tung University, Hsinchu 30010, Taiwan

Department of Chemistry, College of Natural Science, Dire Dawa University, Dire Dawa 1362, Ethiopia

Center of Atomic Initiative for New Materials, National Taiwan University, Taipei 10617, Taiwan

Department of Chemistry, National Taiwan University, Taipei 10617, Taiwan

Institute of Physics, Academia Sinica, Taipei 11529, Taiwan

Nano Science and Technology, Taiwan International Graduate Program, Academia Sinica, Nangang, Taipei 11529, Taiwan

Center for Condensed Matter Sciences, National Taiwan University, Taipei 10617, Taiwan

Division of Natural Science, Center for General Education, Chang Gung University, Taoyuan City 33302, Taiwan

Tabbin Institute for Metallurgical Studies, Tabbin, Helwan 109, Cairo 11421, Egypt

Materials Science Center, National Renewable Energy Laboratory (NREL), Golden, Colorado 80401, United States

Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States

National Synchrotron Radiation Research Center, Hsinchu 30092, Taiwan

Department of Physics, National Taiwan University, Taipei 10617, Taiwan

Funding

Center of Atomic Initiative for New Materials, National Taiwan University · Academia Sinica · Ministry of Science and Technology, Taiwan · National Science and Technology Council

References (55)

Show source-provided references
1. 10.1021/acsenergylett.2c0090810.1021/acsenergylett.2c00908 ↗
2. 10.1021/acsenergylett.0c0197710.1021/acsenergylett.0c01977 ↗
3. 10.1038/s41467-017-02291-910.1038/s41467-017-02291-9 ↗
4. 10.1038/nmat369910.1038/nmat3699 ↗
5. 10.1038/s41586-018-0015-410.1038/s41586-018-0015-4 ↗
6. 10.1016/j.cej.2023.14278610.1016/j.cej.2023.142786 ↗
7. 10.1002/celc.20210019710.1002/celc.202100197 ↗
8. 10.1021/acsenergylett.2c0203210.1021/acsenergylett.2c02032 ↗
9. 10.1002/adfm.20231087310.1002/adfm.202310873 ↗
10. 10.1021/acsenergylett.9b0230210.1021/acsenergylett.9b02302 ↗
11. 10.1021/acsenergylett.0c0258410.1021/acsenergylett.0c02584 ↗
12. 10.1002/aenm.20150027410.1002/aenm.201500274 ↗
13. 10.1002/aenm.20180205710.1002/aenm.201802057 ↗
14. 10.1002/aenm.20200120710.1002/aenm.202001207 ↗
15. 10.1002/adfm.20211239410.1002/adfm.202112394 ↗
16. 10.1039/D2CC00477A10.1039/D2CC00477A ↗
17. 10.1021/jacs.1c0682810.1021/jacs.1c06828 ↗
18. 10.1021/jacs.0c0090910.1021/jacs.0c00909 ↗
19. 10.1021/jacs.2c0266810.1021/jacs.2c02668 ↗
20. 10.1021/acs.chemmater.0c0416410.1021/acs.chemmater.0c04164 ↗
21. 10.1038/s41560-019-0493-010.1038/s41560-019-0493-0 ↗
22. 10.1126/science.192.4244.112710.1126/science.192.4244.1127 ↗
23. 10.1016/j.ensm.2019.12.03310.1016/j.ensm.2019.12.033 ↗
24. 10.1149/1.213285410.1149/1.2132854 ↗
25. 10.1103/PhysRevB.37.369910.1103/PhysRevB.37.3699 ↗
26. 10.1016/j.jpowsour.2010.11.05110.1016/j.jpowsour.2010.11.051 ↗
27. 10.1149/1.209642610.1149/1.2096426 ↗
28. 10.1107/S002188981103897010.1107/S0021889811038970 ↗
29. 10.1016/0927-0256(96)00008-010.1016/0927-0256(96)00008-0 ↗
30. 10.1103/PhysRevB.54.1116910.1103/PhysRevB.54.11169 ↗
31. 10.1103/PhysRevB.50.1795310.1103/PhysRevB.50.17953 ↗
32. 10.1063/1.500610410.1063/1.5006104 ↗
33. 10.1103/PhysRevLett.77.386510.1103/PhysRevLett.77.3865 ↗
34. 10.1016/j.commatsci.2019.03.04910.1016/j.commatsci.2019.03.049 ↗
35. 10.1063/1.481232310.1063/1.4812323 ↗
36. 10.1021/acs.chemmater.2c0148910.1021/acs.chemmater.2c01489 ↗
37. 10.1016/j.mtphys.2022.10088910.1016/j.mtphys.2022.100889 ↗
38. 10.1038/416826a10.1038/416826a ↗
39. 10.1038/s41467-022-28926-010.1038/s41467-022-28926-0 ↗
40. 10.1038/s41467-022-30517-y10.1038/s41467-022-30517-y ↗
41. 10.1021/jp060670c10.1021/jp060670c ↗
42. 10.1021/acssuschemeng.1c0134110.1021/acssuschemeng.1c01341 ↗
43. 10.1002/aenm.20230401810.1002/aenm.202304018 ↗
44. 10.1002/er.359810.1002/er.3598 ↗
45. 10.1016/S0378-7753(02)00310-510.1016/S0378-7753(02)00310-5 ↗
46. 10.1016/j.est.2020.10132910.1016/j.est.2020.101329 ↗
47. 10.1016/j.jpowsour.2013.11.02910.1016/j.jpowsour.2013.11.029 ↗
48. 10.1021/acs.inorgchem.6b0029510.1021/acs.inorgchem.6b00295 ↗
49. 10.1021/ar990125c10.1021/ar990125c ↗
50. 10.1016/j.ccr.2004.03.02010.1016/j.ccr.2004.03.020 ↗
51. 10.1149/2.0081507jes10.1149/2.0081507jes ↗
52. 10.1021/acssuschemeng.1c0819610.1021/acssuschemeng.1c08196 ↗
53. 10.1021/ja901868q10.1021/ja901868q ↗
54. 10.1007/s00269000012910.1007/s002690000129 ↗
55. 10.1021/ja00191a01210.1021/ja00191a012 ↗