Toward a Mechanistic Model of Solid–Electrolyte Interphase Formation and Evolution in Lithium-Ion Batteries
Source abstract
Abstract
The formation of passivation films by interfacial reactions, though critical for applications ranging from advanced alloys to electrochemical energy storage, is often poorly understood. In this work, we explore the formation of an exemplar passivation film, the solid-electrolyte interphase (SEI), which is responsible for stabilizing lithium-ion batteries. Using stochastic simulations based on quantum chemical calculations and data-driven chemical reaction networks, we directly model competition between SEI products at a mechanistic level for the first time. Our results recover the Peled-like separation of the SEI into inorganic and organic domains resulting from rich reactive competition without fitting parameters to experimental inputs. By conducting accelerated simulations at elevated temperature, we track SEI evolution, confirming the postulated reduction of lithium ethylene monocarbonate to dilithium ethylene monocarbonate and H2. These findings furnish fundamental insights into the dynamics of SEI formation and illustrate a path forward toward a predictive understanding of electrochemical passivation.
Source: openalex_inverted_index · Quality: baseline
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
Materials Science Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States
Department of Materials Science and Engineering, University of California, Berkeley, 210 Hearst Memorial Mining Building, Berkeley, California 94720, United States
Department of Chemical and Biomolecular Engineering, University of California, Berkeley, 201 Gilman Hall, Berkeley, California 94720, United States
Energy Storage and Distributed Resources, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States
Department of Chemistry, University of California, Berkeley, 419 Latimer Hall, Berkeley, California 94720, United States
Molecular Foundry, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States
Funding
Basic Energy Sciences · U.S. Department of Energy
References (66)
Show source-provided references
1. 10.1016/j.corsci.2015.08.03810.1016/j.corsci.2015.08.038 ↗
2. 10.1016/j.corsci.2016.05.04110.1016/j.corsci.2016.05.041 ↗
3. 10.1016/j.surfcoat.2018.10.09010.1016/j.surfcoat.2018.10.090 ↗
4. 10.1116/1.212795410.1116/1.2127954 ↗
5. 10.3390/cryst805022610.3390/cryst8050226 ↗
6. 10.1021/acsami.9b1689810.1021/acsami.9b16898 ↗
7. 10.1016/j.solmat.2018.04.02910.1016/j.solmat.2018.04.029 ↗
8. 10.1016/j.mtener.2018.01.00410.1016/j.mtener.2018.01.004 ↗
9. 10.1524/zpch.2009.608610.1524/zpch.2009.6086 ↗
10. 10.1002/adfm.20210093810.1002/adfm.202100938 ↗
11. 10.1116/1.56934010.1116/1.569340 ↗
12. 10.1016/S0300-9440(01)00134-510.1016/S0300-9440(01)00134-5 ↗
13. 10.1063/1.296370710.1063/1.2963707 ↗
14. 10.1016/j.matt.2019.05.01610.1016/j.matt.2019.05.016 ↗
15. 10.1002/aenm.20200229710.1002/aenm.202002297 ↗
16. 10.1016/j.electacta.2011.03.05310.1016/j.electacta.2011.03.053 ↗
17. 10.1021/acsenergylett.7b0035610.1021/acsenergylett.7b00356 ↗
18. 10.1016/j.jmst.2017.11.02110.1016/j.jmst.2017.11.021 ↗
19. 10.1149/2.1081915jes10.1149/2.1081915jes ↗
20. 10.1016/j.carbon.2016.04.00810.1016/j.carbon.2016.04.008 ↗
21. 10.1016/j.scriptamat.2020.06.06510.1016/j.scriptamat.2020.06.065 ↗
22. 10.1002/advs.20150021310.1002/advs.201500213 ↗
23. 10.1149/1.204865910.1149/1.2048659 ↗
24. 10.1021/jp052474w10.1021/jp052474w ↗
25. 10.1016/j.electacta.2010.05.07210.1016/j.electacta.2010.05.072 ↗
26. 10.1021/jp404155y10.1021/jp404155y ↗
27. 10.1038/s41557-019-0304-z10.1038/s41557-019-0304-z ↗
28. 10.1021/jacs.0c0636310.1021/jacs.0c06363 ↗
29. 10.1149/2.1441707jes10.1149/2.1441707jes ↗
30. 10.1149/2.0041906jes10.1149/2.0041906jes ↗
31. 10.1016/j.egyr.2020.02.02210.1016/j.egyr.2020.02.022 ↗
32. 10.1021/ja016452910.1021/ja0164529 ↗
33. 10.1002/qua.2046610.1002/qua.20466 ↗
34. 10.1021/jp210345b10.1021/jp210345b ↗
35. 10.1039/D0CP03286G10.1039/D0CP03286G ↗
36. 10.1039/b925853a10.1039/b925853a ↗
37. 10.1021/am404365r10.1021/am404365r ↗
38. 10.1039/D0SC05647B10.1039/D0SC05647B ↗
39. 10.1021/jacs.1c0580710.1021/jacs.1c05807 ↗
40. 10.1016/j.cplett.2012.08.02210.1016/j.cplett.2012.08.022 ↗
41. 10.1016/j.joule.2019.08.01810.1016/j.joule.2019.08.018 ↗
42. 10.26434/chemrxiv-2021-c2gp3-v210.26434/chemrxiv-2021-c2gp3-v2 ↗
43. 10.1063/1.169679210.1063/1.1696792 ↗
44. 10.1149/1.354852610.1149/1.3548526 ↗
45. 10.1149/2.0241711jes10.1149/2.0241711jes ↗
46. 10.1016/j.electacta.2021.13927210.1016/j.electacta.2021.139272 ↗
47. 10.1021/acsami.1c2048710.1021/acsami.1c20487 ↗
48. 10.1088/2516-1083/ac1a6510.1088/2516-1083/ac1a65 ↗
49. 10.1088/2516-1083/ac389410.1088/2516-1083/ac3894 ↗
50. 10.1021/j100540a00810.1021/j100540a008 ↗
51. 10.2172/96694210.2172/966942 ↗
52. 10.1149/2.0191510jes10.1149/2.0191510jes ↗
53. 10.1016/j.joule.2017.08.00910.1016/j.joule.2017.08.009 ↗
54. 10.1149/2.015301jes10.1149/2.015301jes ↗
55. 10.1149/1.347422510.1149/1.3474225 ↗
56. 10.1016/j.jpowsour.2016.08.01510.1016/j.jpowsour.2016.08.015 ↗
57. 10.1021/acs.chemmater.5b0335810.1021/acs.chemmater.5b03358 ↗
58. 10.1002/cssc.20180007710.1002/cssc.201800077 ↗
59. 10.1016/j.jpowsour.2006.07.07410.1016/j.jpowsour.2006.07.074 ↗
60. 10.1149/1.222103410.1149/1.2221034 ↗
61. 10.1149/1.205477710.1149/1.2054777 ↗
62. 10.1016/0013-4686(94)00221-510.1016/0013-4686(94)00221-5 ↗
63. 10.1149/1.205471810.1149/1.2054718 ↗
64. 10.1149/2.0821910jes10.1149/2.0821910jes ↗
65. 10.1016/j.jpowsour.2013.05.04010.1016/j.jpowsour.2013.05.040 ↗
66. 10.1149/2.1091807jes10.1149/2.1091807jes ↗