DataVXACS Energy LettersPaper
journal article·2025-06-13

Concentration-Dependent Thermodynamics and Kinetics in Lithium-Metal Battery Electrolytes: Implications for Coulombic Efficiency

Christian O. Plaza-Rivera, Daniel Wang, Jason K. Phong, Haldrian Iriawan, Maximiliano Ramirez, Bryce A. Tappan, Louis Ah, Yang Shao-Horn

ACS Energy Letters· Volume 10· Issue 6
Publisher page
Source abstract

Abstract

Lithium (Li)-metal batteries (LMBs) are promising for high-energy applications but are hindered by dendrite formation and unstable interphases. This study investigated Li plating thermodynamics and kinetics as descriptors governing Coulombic efficiency (CE), focusing on lithium bis(fluorosulfonyl)imide in fluoroethylene carbonate and 1,2-dimethoxyethane electrolytes. First, upshifts in Li + /Li potential ( E Li + /Li vs Me 10 Fc), via low donor number solvents and high salt concentrations, correlated with increased CEs. Second, reaction (Δ S Li + Li ) and configurational entropy ( S C ), obtained via Seebeck coefficient and heat capacity measurements, respectively, did not correlate with CE and formed a minority contribution to Li + /Li reaction free energy, revealing the primarily enthalpic origin of the E Li + /Li correlation. Finally, kinetic analyses to examine the balance of exchange current density ( j 0 ) and diffusion ( D Li ) showing lower D Li / j 0 led to higher CE. These CE correlations highlight the combined effects of thermodynamics and kinetics on Li reversibility, informing rational strategies for enhanced performance of LMBs.
Source: openalex_inverted_index · Quality: baseline

Research context

Energy storage

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 Materials Science and Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Department of Mechanical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Department of Chemical Engineering, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Research Laboratory of Electronics, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Department of Chemistry, Massachusetts Institute of Technology, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States

Funding

Bundesministerium f??r Bildung und Forschung · U.S. Department of Energy · Toyota Research Institute · MIT Energy Initiative · Energy Storage Research Alliance ESRA

References (47)

Show source-provided references
1. 10.5796/electrochemistry.84.21010.5796/electrochemistry.84.210 ↗
2. 10.1002/aenm.20200309210.1002/aenm.202003092 ↗
3. 10.1016/j.joule.2021.12.01810.1016/j.joule.2021.12.018 ↗
4. 10.1038/s41560-022-01144-010.1038/s41560-022-01144-0 ↗
5. 10.1021/acsenergylett.9b0038110.1021/acsenergylett.9b00381 ↗
6. 10.1002/adma.20170610210.1002/adma.201706102 ↗
7. 10.1073/pnas.171289511510.1073/pnas.1712895115 ↗
8. 10.1038/s41560-021-00910-w10.1038/s41560-021-00910-w ↗
9. 10.1038/ncomms736210.1038/ncomms7362 ↗
10. 10.1038/s41560-023-01208-910.1038/s41560-023-01208-9 ↗
11. 10.1149/2.0041514jes10.1149/2.0041514jes ↗
12. 10.1021/acsami.9b1194210.1021/acsami.9b11942 ↗
13. 10.1038/ncomms1203210.1038/ncomms12032 ↗
14. 10.1021/ja412807w10.1021/ja412807w ↗
15. 10.1038/ncomms251310.1038/ncomms2513 ↗
16. 10.1149/1945-7111/abd60e10.1149/1945-7111/abd60e ↗
17. 10.5796/electrochemistry.22-0001410.5796/electrochemistry.22-00014 ↗
18. 10.1016/j.chempr.2018.05.00210.1016/j.chempr.2018.05.002 ↗
19. 10.1021/acs.chemrev.9b0053110.1021/acs.chemrev.9b00531 ↗
20. 10.1039/D0EE01446J10.1039/D0EE01446J ↗
21. 10.1016/j.chempr.2019.07.00310.1016/j.chempr.2019.07.003 ↗
22. 10.1038/s41560-023-01280-110.1038/s41560-023-01280-1 ↗
23. 10.31635/ccschem.020.20200034110.31635/ccschem.020.202000341 ↗
24. 10.1021/acsenergylett.4c0062110.1021/acsenergylett.4c00621 ↗
25. 10.1002/celc.20240044410.1002/celc.202400444 ↗
26. 10.1073/pnas.191101711610.1073/pnas.1911017116 ↗
27. 10.1038/s41560-024-01494-x10.1038/s41560-024-01494-x ↗
28. 10.1002/ange.20150914310.1002/ange.201509143 ↗
29. 10.1039/D4FD00038B10.1039/D4FD00038B ↗
30. 10.1021/acs.jpcc.9b0996810.1021/acs.jpcc.9b09968 ↗
31. 10.1021/acsenergylett.4c0214910.1021/acsenergylett.4c02149 ↗
32. 10.1002/advs.20200330110.1002/advs.202003301 ↗
33. 10.1039/D2EE04203G10.1039/D2EE04203G ↗
34. 10.1002/aenm.20170209710.1002/aenm.201702097 ↗
35. 10.1016/j.nanoen.2019.10388110.1016/j.nanoen.2019.103881 ↗
36. 10.1016/j.joule.2019.08.01810.1016/j.joule.2019.08.018 ↗
37. 10.1021/jp991381+10.1021/jp991381+ ↗
38. 10.1039/D4EE02989E10.1039/D4EE02989E ↗
39. 10.1021/acs.jpcc.4c0879010.1021/acs.jpcc.4c08790 ↗
40. 10.1038/s41467-023-38387-810.1038/s41467-023-38387-8 ↗
41. 10.1021/jacs.8b0604710.1021/jacs.8b06047 ↗
42. 10.1021/acs.jpcc.4c0466810.1021/acs.jpcc.4c04668 ↗
43. 10.1021/jacs.0c1058710.1021/jacs.0c10587 ↗
44. 10.1039/C8CP06638H10.1039/C8CP06638H ↗
45. 10.1021/acs.jpcc.8b0603510.1021/acs.jpcc.8b06035 ↗
46. 10.1021/acsenergylett.0c0003110.1021/acsenergylett.0c00031 ↗
47. 10.1149/1.206903310.1149/1.2069033 ↗