journal article·2024-10

Aggregate‐Dominated Dilute Electrolytes with Low‐Temperature‐Resistant Ion‐Conducting Channels for Highly Reversible Na Plating/Stripping

Bingcheng Ge, Jiaojiao Deng, Zhijie Wang, Qinghua Liang, Liang Hu, Xiuyun Ren, Runmin Li, Yuxiao Lin, Yunsong Li, Qingrong Wang, Bin Han, Yonghong Deng, Xiulin Fan, Baohua Li, Guohua Chen, Xiaoliang Yu

Advanced Materials· Volume 36· Issue 41
Publisher page

Abstract

Abstract Developing rechargeable batteries with high power delivery at low temperatures (LT) below 0 °C is significant for cold‐climate applications. Initial anode‐free sodium metal batteries (AFSMBs) promise high LT performances because of the low de‐solvation energy and smaller Stokes radius of Na+, nondiffusion‐limited plating/stripping electrochemistry, and maximized energy density. However, the severe reduction in electrolyte ionic conductivity and formation of unstable solid electrolyte interphase (SEI) hinder their practical applications at LT. In this study, a 2‐methyltetrahydrofuran‐based dilute electrolyte is designed to concurrently achieve an anion‐coordinated solvation structure and impressive ionic conductivity of 3.58 mS cm−1 at −40 °C. The dominant aggregate solvates enable the formation of highly efficient and LT‐resistant Na+ hopping channels in the electrolyte. Moreover, the methyl‐regulated electronic structure in 2‐methyltetrahydrofuran induces gradient decomposition toward an inorganic‐organic bilayer SEI with high Na+ mobility, composition homogeneity, and mechanical robustness. As such, a record‐high Coulombic efficiency beyond 99.9% is achieved even at −40 °C. The as‐constructed AFSMBs sustain 300 cycles with 80% capacity maintained, and a 0.5‐Ah level pouch cell delivers 85% capacity over 180 cycles at −25 °C. This study affords new insights into electrolyte formulation for fast ionic conduction and superior Na reversibility at ultralow temperatures.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Fuel Cells and Related Materials

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

Affiliations

Department of Mechanical Engineering and Research Institute for Smart Energy The Hong Kong Polytechnic University Hong Kong 999077 China

Graphene Composite Research Center College of Chemistry and Environmental Engineering Shenzhen University Shenzhen 518060 China

Department of Applied Physics the Hong Kong Polytechnic University Hong Kong 999077 China

Key Laboratory of Rare Earth Ganjiang Innovation Academy Chinese Academy of Sciences Ganzhou Jiangxi 341000 China

School of Physics and Electronic Engineering Jiangsu Normal University Xuzhou 221116 China

Zhejiang Laboratory Hangzhou 311100 China

Department of Materials Science and Engineering School of Innovation and Entrepreneurship Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and Technology Shenzhen 518055 China

State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering Zhejiang University Hangzhou China

Tsinghua Shenzhen International Graduate School Tsinghua University Shenzhen 518055 China

School of Energy and Environment City University of Hong Kong Kowloon Hong Kong China

Funding

National Natural Science Foundation of China · Innovation and Technology Fund · Chinese Academy of Sciences · Shenzhen Science and Technology Innovation Program · Basic and Applied Basic Research Foundation of Guangdong Province · Natural Science Foundation of Jiangxi Province · China Academy of Chinese Medical Sciences

References (60)

Show source-provided references
1. 10.1002/adma.20180056110.1002/adma.201800561 ↗
2. 10.1038/s41467-020-19991-410.1038/s41467-020-19991-4 ↗
3. 10.1002/aenm.20200197210.1002/aenm.202001972 ↗
4. Hubble D. · Environ. Sci. · 2022 · 15 · 550
5. 10.1016/j.etran.2021.10014510.1016/j.etran.2021.100145 ↗
6. 10.1021/acsenergylett.4c0011310.1021/acsenergylett.4c00113 ↗
7. 10.1038/nature1650210.1038/nature16502 ↗
8. 10.1016/j.enconman.2018.12.05110.1016/j.enconman.2018.12.051 ↗
9. 10.1038/s41560-021-00783-z10.1038/s41560-021-00783-z ↗
10. 10.1038/s41560-024-01527-510.1038/s41560-024-01527-5 ↗
11. 10.1039/D1CS00948F10.1039/D1CS00948F ↗
12. 10.1021/acsenergylett.2c0252910.1021/acsenergylett.2c02529 ↗
13. 10.1016/j.isci.2023.10598210.1016/j.isci.2023.105982 ↗
14. 10.1016/j.chempr.2019.05.02610.1016/j.chempr.2019.05.026 ↗
15. 10.1002/aenm.20200385410.1002/aenm.202003854 ↗
16. 10.1002/smll.20210113710.1002/smll.202101137 ↗
17. 10.1021/jacs.1c0611510.1021/jacs.1c06115 ↗
18. 10.1039/D4TA01400F10.1039/D4TA01400F ↗
19. 10.1038/s41467-022-32606-410.1038/s41467-022-32606-4 ↗
20. 10.1002/jcc.2696310.1002/jcc.26963 ↗
21. 10.1021/acsnano.3c1287710.1021/acsnano.3c12877 ↗
22. 10.1002/aenm.20200309210.1002/aenm.202003092 ↗
23. 10.1002/aenm.202304414230441410.1002/aenm.2023044142304414 ↗
24. 10.1021/acs.nanolett.1c0483510.1021/acs.nanolett.1c04835 ↗
25. 10.1073/pnas.231691412110.1073/pnas.2316914121 ↗
26. 10.1021/acsenergylett.1c0239110.1021/acsenergylett.1c02391 ↗
27. 10.1002/agt2.15310.1002/agt2.153 ↗
28. 10.1016/j.nanoen.2016.09.01310.1016/j.nanoen.2016.09.013 ↗
29. 10.1007/s12598-020-01576-110.1007/s12598-020-01576-1 ↗
30. 10.1021/jacs.3c1113410.1021/jacs.3c11134 ↗
31. 10.1002/anie.20240053910.1002/anie.202400539 ↗
32. 10.1038/s41586-024-07045-410.1038/s41586-024-07045-4 ↗
33. Ponrouch A. · Environ Sci · 2012 · 5 · 8572
34. 10.1021/acscentsci.5b0032810.1021/acscentsci.5b00328 ↗
35. 10.1002/aenm.202304321230432110.1002/aenm.2023043212304321 ↗
36. 10.1039/D3CS00151B10.1039/D3CS00151B ↗
37. 10.1002/anie.20201148210.1002/anie.202011482 ↗
38. 10.1021/acsmaterialslett.3c0116410.1021/acsmaterialslett.3c01164 ↗
39. 10.1016/j.ensm.2022.05.00510.1016/j.ensm.2022.05.005 ↗
40. 10.1002/anie.20201424110.1002/anie.202014241 ↗
41. 10.1039/D1TA00842K10.1039/D1TA00842K ↗
42. 10.1002/anie.20211255010.1002/anie.202112550 ↗
43. 10.1016/j.joule.2024.01.01010.1016/j.joule.2024.01.010 ↗
44. 10.1016/j.electacta.2019.02.11010.1016/j.electacta.2019.02.110 ↗
45. 10.1103/PhysRevB.98.03543410.1103/PhysRevB.98.035434 ↗
46. 10.1149/1945-7111/ac1cc310.1149/1945-7111/ac1cc3 ↗
47. 10.1002/adfm.20220460910.1002/adfm.202204609 ↗
48. 10.1002/adma.20230084110.1002/adma.202300841 ↗
49. 10.1016/j.jcis.2023.12.01210.1016/j.jcis.2023.12.012 ↗
50. 10.1021/jacs.3c1227210.1021/jacs.3c12272 ↗
51. 10.1021/acsenergylett.3c0005210.1021/acsenergylett.3c00052 ↗
52. Park S.‐J. · 2011 · 1
53. 10.1002/adfm.20200489110.1002/adfm.202004891 ↗
54. 10.1002/adma.20210057410.1002/adma.202100574 ↗
55. 10.1002/aenm.20220039810.1002/aenm.202200398 ↗
56. 10.1038/s41560-018-0097-010.1038/s41560-018-0097-0 ↗
57. 10.1149/2.0881803jes10.1149/2.0881803jes ↗
58. 10.1002/anie.20220647110.1002/anie.202206471 ↗
59. 10.1002/adfm.20211239910.1002/adfm.202112399 ↗
60. 10.1038/s41560-021-00910-w10.1038/s41560-021-00910-w ↗