Relationship of the Molecular Structure and Transport Properties of Imide-Based Lithium Salts of “Acetonitrile/Water-in-Salt” Electrolytes

Xinyi Liu; Shao-Chun Lee; Soenke Seifert; Randall E. Winans; Y Z; Tao Li

doi:10.1021/acs.chemmater.3c01148

journal article·2023-08-22Open access

Relationship of the Molecular Structure and Transport Properties of Imide-Based Lithium Salts of “Acetonitrile/Water-in-Salt” Electrolytes

Xinyi Liu, Shao-Chun Lee, Soenke Seifert, Randall E. Winans, Y Z, Tao Li

Chemistry of Materials· Volume 35· Issue 16

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Source abstract

Abstract

“Water-in-salt” (WIS) electrolytes exhibit excellent safety and electrochemical performance. However, they possess high concentrations, relatively low diffusion coefficient, and high viscosity. “Acetonitrile/water in salt” (AWIS) electrolytes can overcome the disadvantages of WIS electrolytes. Under relatively low concentrations, AWIS electrolytes show good electrochemical performance comparable to WIS electrolytes and low conductivity. Herein, we investigate the relationship between the solvation structures and the transport properties using small-angle X-ray scattering and molecular dynamics simulation. We observed two solvation behaviors of AWIS: anions dissolved in acetonitrile forming small acetonitrile/anion clusters and additional water further dissolving the small acetonitrile/anion clusters. The introduction of acetonitrile weakens the water–solute interaction and enhances the cation–anion interaction, which results in an enhanced dynamical slowdown as the concentration increases. This work provides molecular-level understanding of the connection between two-stage solvation structures and transport properties for imide-based lithium salt solutions.

Source: openalex_inverted_index · Quality: baseline

Research context

Energy storage

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Membrane-based Ion Separation Techniques

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

Affiliations

Department of Chemistry and Biochemistry, Northern Illinois University, DeKalb, Illinois 60115, United States

Department of Nuclear, Plasma and Radiological Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States

Beckman Institute for Advanced Science and Technology, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States

X-ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States

Joint Center for Energy Storage Research, Argonne National Laboratory, Lemont, Illinois 60439, United States

Department of Electrical and Computer Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States

Department of Nuclear Engineering and Radiological Sciences, University of Michigan, Ann Arbor, Michigan 48109, United States

Funding

Basic Energy Sciences · Division of Chemical, Bioengineering, Environmental, and Transport Systems

References (40)

Show source-provided references

1. 10.1021/ja412807w10.1021/ja412807w ↗

2. 10.1149/ma2016-03/2/106310.1149/ma2016-03/2/1063 ↗

3. 10.1021/jacs.7b1068810.1021/jacs.7b10688 ↗

4. 10.1149/ma2015-01/15/115510.1149/ma2015-01/15/1155 ↗

5. 10.1038/s41560-019-0336-z10.1038/s41560-019-0336-z ↗

6. 10.1149/2.0041514jes10.1149/2.0041514jes ↗

7. 10.1126/science.aab159510.1126/science.aab1595 ↗

8. 10.34133/2021/736842010.34133/2021/7368420 ↗

9. 10.1016/j.ensm.2021.12.01610.1016/j.ensm.2021.12.016 ↗

10. 10.1021/acs.jpcb.1c0218910.1021/acs.jpcb.1c02189 ↗

11. 10.1002/aenm.20200282110.1002/aenm.202002821 ↗

12. 10.1149/1945-7111/abf97510.1149/1945-7111/abf975 ↗

13. 10.1002/aenm.20170263010.1002/aenm.201702630 ↗

14. 10.1002/chem.20170442010.1002/chem.201704420 ↗

15. 10.1039/c5ee02702k10.1039/c5ee02702k ↗

16. 10.1016/j.ensm.2016.10.00210.1016/j.ensm.2016.10.002 ↗

17. 10.1016/j.electacta.2008.03.01210.1016/j.electacta.2008.03.012 ↗

18. 10.1021/acs.jpcb.1c0758110.1021/acs.jpcb.1c07581 ↗

19. 10.1021/acsenergylett.1c0201210.1021/acsenergylett.1c02012 ↗

20. 10.1039/c8ee01040d10.1039/c8ee01040d ↗

21. 10.1021/acsnano.7b0566410.1021/acsnano.7b05664 ↗

22. 10.1039/d1cp02006d10.1039/d1cp02006d ↗

23. 10.1021/acs.jpcb.0c0351610.1021/acs.jpcb.0c03516 ↗

24. 10.1021/acs.jpcc.0c0218710.1021/acs.jpcc.0c02187 ↗

25. 10.1021/acs.jpcc.9b1080710.1021/acs.jpcc.9b10807 ↗

26. 10.1021/acsenergylett.0c0255910.1021/acsenergylett.0c02559 ↗

27. 10.1021/acs.jpclett.9b0349510.1021/acs.jpclett.9b03495 ↗

28. 10.1021/acsenergylett.1c0239110.1021/acsenergylett.1c02391 ↗

29. 10.1002/batt.20200023710.1002/batt.202000237 ↗

30. 10.1002/cphc.20200015310.1002/cphc.202000153 ↗

31. 10.1021/acs.jpcc.1c0935210.1021/acs.jpcc.1c09352 ↗

32. 10.1016/0022-3093(74)90030-110.1016/0022-3093(74)90030-1 ↗

33. 10.1021/acs.chemmater.2c0365410.1021/acs.chemmater.2c03654 ↗

34. 10.1021/acs.jpcb.0c0119710.1021/acs.jpcb.0c01197 ↗

35. 10.1007/s00214-012-1129-710.1007/s00214-012-1129-7 ↗

36. 10.1021/ja962176010.1021/ja9621760 ↗

37. 10.1021/j100308a03810.1021/j100308a038 ↗

38. 10.1006/jcph.1995.103910.1006/jcph.1995.1039 ↗

39. 10.1016/j.cpc.2018.03.00510.1016/j.cpc.2018.03.005 ↗

40. 10.1016/0263-7855(96)00018-510.1016/0263-7855(96)00018-5 ↗