journal article·2025-04-11Open access

Multiscale Defect Regulation of Cobalt-Free Layered Oxides for High-Energy and Long-Lasting Cathodes

Kun-Hee Ko, Hyeokjun Park, Jaesang Yoon, Seok Hyun Song, Eugene Choi, Sungjae Seo, Jaesub Kwon, Sunyoung Lee, Jaehoon Heo, Sangwook Han, Jooha Park, Wonju Kim, Yong-Tae Kim, Jongwoo Lim, Yun Seog Lee, Hyungsub Kim, Kisuk Kang

ACS Energy Letters· Volume 10· Issue 4

Abstract

High Resolution Image Download MS PowerPoint Slide Reducing the reliance on cobalt in electrode chemistry is a promising step toward more sustainable and cost-effective lithium-ion batteries. However, the elimination of cobalt in layered oxides generally results in a significant decrease in capacity and/or a compromised cycle stability. Herein, we show that these intertwined issues of the cobaltless systems can be remedied by meticulously tailoring inherent defects induced at multiscale. It is demonstrated that a simple excess incorporation of lithium in the structure can effectively reduce the cation disorder and unexpectedly alter the microstructure forming routes, thereby enhancing electro-chemo-mechanical stabilities of layered cathodes. Our investigations reveal that this surplus lithium facilitates topotactic lithiation of precursors during calcination, rendering mechanically robust particles with fewer nanoporous defects and reduced cation disorder. Defect-regulated cobalt-free layered oxides successfully deliver a reversible capacity of 189 mAh g –1 at 0.5C with a retention of ∼85% after 300 cycles under commercial-level electrode loading.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Advancements in Battery Materials · Extraction and Separation Processes · Advanced Battery Materials and Technologies

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

Affiliations

Department of Materials Science and Engineering, and Institute for Rechargeable Battery Innovations, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea

Interdisciplinary Materials Measurement Institute, Korea Research Institute of Standards and Science (KRISS), 267 Gajeong-ro, Yuseong-gu, Daejeon 34113, Republic of Korea

Department of Materials Science and Engineering

Korea University

SDI R&D Center, SAMSUNG SDI CO., LTD., 130 Samsung-ro, Yeongtong-gu, Suwon-si, Gyeonggi-do 16678, Republic of Korea

Neutron Science Center

Korea Atomic Energy Research Institute (KAERI)

Department of Mechanical Engineering, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea

Department of Chemistry, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea

Pohang University of Science and Technology (POSTECH)

Institute of Engineering Research, College of Engineering, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea

Center for Nanoparticle Research, Institute of Basic Science, Seoul National University, 1 Gwanak-ro, Gwanak-gu, Seoul 08826, Republic of Korea

School of Chemical and Biological Engineering, and Institute of Chemical Process

Seoul National University

Funding

National Research Foundation of Korea · Chung Mong-Koo Foundation · Samsung SDI

References (64)

Show source-provided references
1. 10.1038/s41560-019-0513-010.1038/s41560-019-0513-0 ↗
2. 10.1002/aenm.20190386410.1002/aenm.201903864 ↗
3. 10.1016/S0378-7753(99)00221-910.1016/S0378-7753(99)00221-9 ↗
4. 10.1016/j.jpowsour.2013.01.06310.1016/j.jpowsour.2013.01.063 ↗
5. 10.1039/D0EE02511A10.1039/D0EE02511A ↗
6. 10.1002/aenm.20170202810.1002/aenm.201702028 ↗
7. 10.1016/j.exis.2019.05.01810.1016/j.exis.2019.05.018 ↗
8. 10.1149/1.171821110.1149/1.1718211 ↗
9. 10.1021/cm047779m10.1021/cm047779m ↗
10. 10.1021/jp054226610.1021/jp0542266 ↗
11. 10.1126/sciadv.ado447210.1126/sciadv.ado4472 ↗
12. 10.1039/D0EE03581E10.1039/D0EE03581E ↗
13. 10.1021/acs.chemmater.1c0332210.1021/acs.chemmater.1c03322 ↗
14. 10.1021/ja050697u10.1021/ja050697u ↗
15. 10.1016/j.nanoen.2018.04.02010.1016/j.nanoen.2018.04.020 ↗
16. 10.1126/science.112215210.1126/science.1122152 ↗
17. 10.1103/PhysRevB.74.09410510.1103/PhysRevB.74.094105 ↗
18. 10.1126/science.aba916810.1126/science.aba9168 ↗
19. 10.1002/aenm.20130078710.1002/aenm.201300787 ↗
20. 10.1038/s41560-021-00776-y10.1038/s41560-021-00776-y ↗
21. 10.1039/D0EE03774E10.1039/D0EE03774E ↗
22. 10.1021/acsami.0c1254110.1021/acsami.0c12541 ↗
23. 10.1149/2.1751713jes10.1149/2.1751713jes ↗
24. 10.1021/acsenergylett.3c0132210.1021/acsenergylett.3c01322 ↗
25. 10.1002/aenm.20230153010.1002/aenm.202301530 ↗
26. 10.1039/D1EE02898G10.1039/D1EE02898G ↗
27. 10.1038/s41557-022-00915-210.1038/s41557-022-00915-2 ↗
28. 10.1002/adfm.20230665410.1002/adfm.202306654 ↗
29. 10.1002/adfm.20190024710.1002/adfm.201900247 ↗
30. 10.1021/am403684z10.1021/am403684z ↗
31. 10.1021/acs.jpcc.7b0636310.1021/acs.jpcc.7b06363 ↗
32. 10.1016/j.ensm.2020.08.01310.1016/j.ensm.2020.08.013 ↗
33. 10.1021/cm052704j10.1021/cm052704j ↗
34. 10.1021/acs.inorgchem.0c0276610.1021/acs.inorgchem.0c02766 ↗
35. 10.1149/1945-7111/ac24ba10.1149/1945-7111/ac24ba ↗
36. 10.1016/0921-4526(93)90108-I10.1016/0921-4526(93)90108-I ↗
37. 10.3390/nano1004075910.3390/nano10040759 ↗
38. 10.1016/j.electacta.2017.10.10110.1016/j.electacta.2017.10.101 ↗
39. 10.1016/j.jallcom.2018.09.28610.1016/j.jallcom.2018.09.286 ↗
40. 10.1002/anie.20200743610.1002/anie.202007436 ↗
41. 10.1016/j.jpowsour.2020.22836910.1016/j.jpowsour.2020.228369 ↗
42. 10.1002/adfm.20210879010.1002/adfm.202108790 ↗
43. 10.33961/jecst.2022.0044410.33961/jecst.2022.00444 ↗
44. 10.33961/jecst.2023.0029010.33961/jecst.2023.00290 ↗
45. 10.1039/D3TA02784H10.1039/D3TA02784H ↗
46. 10.1007/s11581-021-04204-910.1007/s11581-021-04204-9 ↗
47. 10.33961/jecst.2019.0052810.33961/jecst.2019.00528 ↗
48. 10.1038/s41560-023-01233-810.1038/s41560-023-01233-8 ↗
49. 10.1039/C3EE42704H10.1039/C3EE42704H ↗
50. 10.1021/acs.chemmater.7b0526910.1021/acs.chemmater.7b05269 ↗
51. 10.1149/2.0581903jes10.1149/2.0581903jes ↗
52. 10.1021/acsaem.0c0318710.1021/acsaem.0c03187 ↗
53. 10.1007/s00466-012-0724-810.1007/s00466-012-0724-8 ↗
54. 10.1002/advs.20200036210.1002/advs.202000362 ↗
55. 10.1021/acsnano.9b0504710.1021/acsnano.9b05047 ↗
56. 10.1002/aenm.20247000910.1002/aenm.202470009 ↗
57. 10.1002/adma.20160127310.1002/adma.201601273 ↗
58. 10.1021/acsenergylett.2c0100910.1021/acsenergylett.2c01009 ↗
59. 10.1021/acs.chemmater.9b0351510.1021/acs.chemmater.9b03515 ↗
60. 10.1016/0001-6160(53)90006-610.1016/0001-6160(53)90006-6 ↗
61. 10.1038/s41560-019-0338-x10.1038/s41560-019-0338-x ↗
62. 10.1038/s41560-021-00792-y10.1038/s41560-021-00792-y ↗
63. 10.1093/nsr/nwac22610.1093/nsr/nwac226 ↗
64. 10.1021/acsami.8b0700410.1021/acsami.8b07004 ↗