journal article·2024-11-08

Oxygen Vacancy-Induced Directional Ordering of Li-Ion Pathways for Enhanced Ion-Conducting Solid Electrolytes

Hyeon-Ah Ju, Eun-Byeol Park, Jaejin Hwang, Young-Hoon Kim, Min-Hyoung Jung, Min-Ji Yang, Seon Je Kim, Jaehan Lee, In Kim, Yoo-Shin Kim, Songhun Yoon, Jae Hyuck Jang, Hu Young Jeong, Jaekwang Lee, Jae-Hyun Shim, Young-Min Kim

ACS Energy Letters· Volume 9· Issue 11
Publisher page

Abstract

Defects in perovskite oxide solid electrolytes (SEs) impact Li-ion conductivity. However, the role of oxygen vacancies (V o ) in transport behavior has been less explored. Herein, our study elucidates the microscopic origin of the role of V o in enhancing the total ionic conductivity of a prototype lithium lanthanum titanate while maintaining its insulating properties. Scanning transmission electron microscopy and theoretical calculations reveal that the presence of V o significantly lowers the activation energy of Li-ion migration. The V o is revealed to be preferentially aligned parallel to c -planes and causes modulated lattice expansion in an alternating manner, resulting in easy directional Li-ion transport. The effect of V o -assisted Li-ion transport is optimized through the hierarchical rearrangement of structural features at multiple length scales close to the direction of the V o arrays. Our results offer novel insights into the microscopic origins of superior ion conductivity facilitated by V o, contributing to the design of high-performance SEs.
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Research context

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Advanced battery technologies research

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

Affiliations

Department of Energy Science

Sungkyunkwan University

Department of Physics

Pusan National University

Department of Battery Science and Engineering

Dongshin University

Vinfast Trading and Production JSC, Symphony Building, Chu Huy Man Street, Phuc Loi Commune, Long Bien District, Hanoi 58245, Vietnam

Harvard John A. Paulson School of Engineering and Applied Science

Harvard University

TDL Co., Ltd., 18-6, Hwangdong 3-gil, Naju-si, Jeollanam-do 58327, Republic of Korea

School of Integrative Engineering

Chung-Ang University

Center for Scientific Instrumentation

Korea Basic Science Institute

Graduate School of Semiconductor Materials and Devices Engineering

Ulsan National Institute of Science and Technology (UNIST)

Center for 2D Quantum Heterostructures

Institute for Basic Science (IBS)

Funding

National Research Foundation of Korea · Korea Institute of Energy Technology Evaluation and Planning · Institute for Basic Science · Jeonnam Techno Park

References (42)

Show source-provided references
1. International Energy Agency. · 202010.1787/d394399e-en ↗
2. 10.1021/acsenergylett.0c0197710.1021/acsenergylett.0c01977 ↗
3. 10.1016/j.jpowsour.2021.22991910.1016/j.jpowsour.2021.229919 ↗
4. 10.1016/j.chempr.2018.11.01310.1016/j.chempr.2018.11.013 ↗
5. 10.1038/s41578-019-0165-510.1038/s41578-019-0165-5 ↗
6. 10.1021/acs.nanolett.2c0165510.1021/acs.nanolett.2c01655 ↗
7. 10.1039/c4ee00382a10.1039/c4ee00382a ↗
8. 10.1016/j.jpowsour.2014.11.13910.1016/j.jpowsour.2014.11.139 ↗
9. 10.1016/j.pmatsci.2017.04.00910.1016/j.pmatsci.2017.04.009 ↗
10. 10.1016/j.joule.2018.07.00910.1016/j.joule.2018.07.009 ↗
11. 10.1002/aenm.20160005310.1002/aenm.201600053 ↗
12. 10.1088/0034-4885/67/7/R0510.1088/0034-4885/67/7/R05 ↗
13. 10.1021/cm304135710.1021/cm3041357 ↗
14. 10.1039/C8EE01053F10.1039/C8EE01053F ↗
15. 10.34133/energymatadv.001510.34133/energymatadv.0015 ↗
16. 10.1021/acs.chemrev.5b0056310.1021/acs.chemrev.5b00563 ↗
17. 10.1021/acs.chemmater.1c0234510.1021/acs.chemmater.1c02345 ↗
18. 10.1002/ese3.116310.1002/ese3.1163 ↗
19. 10.1016/j.jpowsour.2021.22979610.1016/j.jpowsour.2021.229796 ↗
20. 10.1039/C3TA13726K10.1039/C3TA13726K ↗
21. 10.1021/ja044922410.1021/ja0449224 ↗
22. 10.1039/b614345h10.1039/b614345h ↗
23. 10.1016/S0167-2738(00)00761-X10.1016/S0167-2738(00)00761-X ↗
24. 10.1016/j.ssi.2006.08.01210.1016/j.ssi.2006.08.012 ↗
25. 10.1006/jssc.2002.956010.1006/jssc.2002.9560 ↗
26. 10.1021/cm030051610.1021/cm0300516 ↗
27. 10.1186/s40543-018-0142-410.1186/s40543-018-0142-4 ↗
28. 10.1038/nmat339310.1038/nmat3393 ↗
29. 10.1016/j.mtphys.2021.10034710.1016/j.mtphys.2021.100347 ↗
30. 10.1016/j.mtphys.2020.10030210.1016/j.mtphys.2020.100302 ↗
31. 10.1103/PhysRevLett.109.06570210.1103/PhysRevLett.109.065702 ↗
32. 10.1038/nmat405810.1038/nmat4058 ↗
33. 10.1103/PhysRevB.98.09410210.1103/PhysRevB.98.094102 ↗
34. 10.1111/jace.1330710.1111/jace.13307 ↗
35. 10.1039/D0NH00340A10.1039/D0NH00340A ↗
36. 10.1080/09500839717987710.1080/095008397179877 ↗
37. 10.1002/admi.20190194410.1002/admi.201901944 ↗
38. 10.1103/PhysRevB.85.20120110.1103/PhysRevB.85.201201 ↗
39. 10.1002/adma.20120066710.1002/adma.201200667 ↗
40. 10.1021/acsnano.5b0323210.1021/acsnano.5b03232 ↗
41. 10.1038/nmat295710.1038/nmat2957 ↗
42. 10.1021/acs.nanolett.0c0351610.1021/acs.nanolett.0c03516 ↗