journal article·2023-04

Reinforcing Native Solid‐Electrolyte Interphase Layers via Electrolyte‐Swellable Soft‐Scaffold for Lithium Metal Anode

Jaehyeong Bae, Keonwoo Choi, Hyunsub Song, Do Heung Kim, Doo Young Youn, Su‐Ho Cho, Dogyeong Jeon, Jiyoung Lee, Junyoung Lee, Wontae Jang, Changhyeon Lee, Youson Kim, Chanhoon Kim, Ji‐Won Jung, Sung Gap Im, Il‐Doo Kim

Advanced Energy Materials· Volume 13· Issue 16
Publisher page

Abstract

Abstract The lithium metal anode is notoriously unstable and reactive to electrolytes, forming brittle solid‐electrolyte interphase (SEI) layers with uneven distribution, exacerbating Li dendrites that ultimately limit the battery life. Here, this work passivates Li metal with electrolyte‐swellable polymer nanolayers deposited monolithically by the initiated chemical vapor deposition (iCVD) to reinforce the native SEI layers and stabilize their interface. The 100 nm iCVD poly(dimethylaminomethyl styrene) (pDMAMS) layer is swelled by 264% under a carbonate electrolyte, establishing the electrolyte‐filled soft scaffold for Li‐ion transport. Notably, the solvogel accommodates homogeneous Li2O‐free and Li2CO3‐rich native SEI layers, providing a record‐high Li‐ion transference number of 0.95 and ionic conductivity of 6.54 mS cm−1. The developed pDMAMS‐Li anodes extend the cycle life by 550% in Li–Li symmetric cells and 600% in LiNi0.6Mn0.2Co0.2O2 full cells compared to pristine Li metal. The mechanistic details of the swollen‐soft‐scaffold strategy are elucidated by depth profile analysis of the pDMAMS homopolymer compared to pDMAMS/electrolyte‐phobic copolymers, providing new insights to manage the interface of liquid‐state electrolyte and solid‐state Li metal by using a novel class of bifunctional solvogel.
Source: crossref · Quality: baseline

Research context

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

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

Affiliations

Department of Materials Science and Engineering Korea Advanced Institute of Science and Technology (KAIST) 291 Daehak‐ro Yuseong‐gu Daejeon 34141 Republic of Korea

Department of Chemical Engineering College of Engineering Kyung Hee University 1732, Deogyeong‐daero, Giheung‐gu Yongin‐si Gyeonggi‐do 17104 Republic of Korea

John A. Paulson School of Engineering and Applied Science Harvard University Cambridge MA 02138 USA

Department of Chemical and Biomolecular Engineering Korea Advanced Institute of Science and Technology (KAIST) 291 Daehak‐ro Yuseong‐gu Daejeon 34141 Republic of Korea

Sustainable Technology and Wellness R&D Group Korea Institute of Industrial Technology (KITECH) 102 Jejudaehak‐ro Jeju‐si Jeju‐do 63243 Republic of Korea

School of Materials Science and Engineering University of Ulsan 12 Techno saneop‐ro 55 beon‐gil Nam‐gu Ulsan 44776 Republic of Korea

KAIST institute for NanoCentury KAIST 291 Daehak‐ro Yuseong‐gu Daejeon 34141 Republic of Korea

Funding

National Research Foundation of Korea · KAIST Wearable Platform Material Technology Center

References (61)

Show source-provided references
1. 10.1038/nnano.2017.1610.1038/nnano.2017.16 ↗
2. 10.1021/acs.chemrev.7b0011510.1021/acs.chemrev.7b00115 ↗
3. Shriver D. · 2014
4. 10.1002/sus2.3710.1002/sus2.37 ↗
5. 10.1016/j.apsusc.2020.14798310.1016/j.apsusc.2020.147983 ↗
6. 10.1088/1361-6528/ac17fe10.1088/1361-6528/ac17fe ↗
7. 10.1016/j.scib.2020.02.02210.1016/j.scib.2020.02.022 ↗
8. 10.1002/anie.20210795710.1002/anie.202107957 ↗
9. 10.1021/acsenergylett.1c0152110.1021/acsenergylett.1c01521 ↗
10. 10.1002/adma.20160375510.1002/adma.201603755 ↗
11. 10.1002/adfm.20210439510.1002/adfm.202104395 ↗
12. 10.1002/aenm.20210038710.1002/aenm.202100387 ↗
13. 10.1039/C9TA05804D10.1039/C9TA05804D ↗
14. 10.1038/s41565-018-0061-y10.1038/s41565-018-0061-y ↗
15. 10.1038/s41560-018-0237-610.1038/s41560-018-0237-6 ↗
16. 10.1002/adma.20150452610.1002/adma.201504526 ↗
17. 10.1016/j.jpowsour.2015.07.02710.1016/j.jpowsour.2015.07.027 ↗
18. 10.1038/s41586-021-04209-410.1038/s41586-021-04209-4 ↗
19. 10.1016/j.xcrp.2020.10011910.1016/j.xcrp.2020.100119 ↗
20. 10.5796/electrochemistry.84.85410.5796/electrochemistry.84.854 ↗
21. 10.1016/j.matt.2020.10.02110.1016/j.matt.2020.10.021 ↗
22. 10.1126/science.abi870310.1126/science.abi8703 ↗
23. 10.1007/s13233-020-8028-x10.1007/s13233-020-8028-x ↗
24. 10.1021/acsaem.0c0097010.1021/acsaem.0c00970 ↗
25. 10.1016/j.matt.2021.09.02510.1016/j.matt.2021.09.025 ↗
26. 10.1021/acsami.5b0572010.1021/acsami.5b05720 ↗
27. 10.1002/adem.20170062210.1002/adem.201700622 ↗
28. 10.1038/nmat423710.1038/nmat4237 ↗
29. 10.1039/C5TC03007B10.1039/C5TC03007B ↗
30. 10.1007/s10853-018-2971-310.1007/s10853-018-2971-3 ↗
31. 10.1039/C5TA03471J10.1039/C5TA03471J ↗
32. 10.1039/D2MA00215A10.1039/D2MA00215A ↗
33. 10.3390/pr403003210.3390/pr4030032 ↗
34. 10.1038/s41598-019-42050-y10.1038/s41598-019-42050-y ↗
35. 10.1038/s41467-019-12423-y10.1038/s41467-019-12423-y ↗
36. 10.1021/ac010887x10.1021/ac010887x ↗
37. Abbott S. · 2017
38. 10.1201/978020375261610.1201/9780203752616 ↗
39. 10.1021/bm100498a10.1021/bm100498a ↗
40. 10.1039/D1DT03532K10.1039/D1DT03532K ↗
41. 10.1016/j.esci.2022.06.00510.1016/j.esci.2022.06.005 ↗
42. 10.1021/acs.langmuir.8b0062410.1021/acs.langmuir.8b00624 ↗
43. 10.1021/acsabm.0c0084410.1021/acsabm.0c00844 ↗
44. 10.1021/ma050394k10.1021/ma050394k ↗
45. 10.1039/C7TA00371D10.1039/C7TA00371D ↗
46. 10.1016/0167-2738(88)90304-910.1016/0167-2738(88)90304-9 ↗
47. 10.1038/nenergy.2017.1210.1038/nenergy.2017.12 ↗
48. 10.1021/acs.chemmater.0c0421810.1021/acs.chemmater.0c04218 ↗
49. 10.1002/adfm.20170583810.1002/adfm.201705838 ↗
50. 10.1039/D1EE00508A10.1039/D1EE00508A ↗
51. 10.1038/s41467-020-15355-010.1038/s41467-020-15355-0 ↗
52. 10.1002/advs.20150021310.1002/advs.201500213 ↗
53. 10.1073/pnas.191101711610.1073/pnas.1911017116 ↗
54. 10.1002/adma.20210040410.1002/adma.202100404 ↗
55. 10.1039/D1RE00191D10.1039/D1RE00191D ↗
56. 10.1038/s41560-020-0577-x10.1038/s41560-020-0577-x ↗
57. 10.1021/acs.jpcc.6b0644610.1021/acs.jpcc.6b06446 ↗
58. 10.1039/C9TA05063A10.1039/C9TA05063A ↗
59. 10.1002/aenm.20220033710.1002/aenm.202200337 ↗
60. 10.1149/2.0391902jes10.1149/2.0391902jes ↗
61. 10.1149/1.213311210.1149/1.2133112 ↗