journal article·2025-04-11

Elucidating Charge Carrier Solvation in Biredox Eutectic Electrolytes for Nonaqueous Symmetrical Organic Redox Flow Batteries

Chengxin Peng, Yunjie Cao, Wanghao Li, Yue Liu, Zhou Zhang, Liang Wang, Wenjing Tang, Ting Yi, Shixue Dou, Yu Zhao

ACS Energy Letters· Volume 10· Issue 4
Publisher page

Abstract

Charge carrier solvation is crucial for mass transfer rates and redox kinetics of redox couples in organic redox flow batteries (ORFBs), yet it remains underexplored. This study employs molecular dynamics simulations to investigate charge carrier solvation in biredox eutectic electrolytes (BEEs) under diverse solvent and salt conditions. Results demonstrate that acetonitrile (ACN) molecules preferentially occupy the primary solvation shell of the bis(trifluoromethanesulfonimide) anions (TFSI – ) in the catholyte and the tetrabutylammonium cations (TBA + ) in the anolyte, forming charge carrier solvation, thus decoupling the molecular interactions within the BEEs and accelerating the redox kinetics in ORFBs. With an optimized ACN-TBATFSI electrolyte, a prototype symmetrical flow cell can achieve a high output voltage of 2.35 V, high material utilization of 93%, and stable cyclability with a capacity retention rate of 99.97% per cycle after 1200 cycles. This work highlights the potential of modulating the charge carrier solvation to enhance the electrochemical performance of ORFBs.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Advanced battery technologies research · Electrochemical Analysis and Applications · Supercapacitor Materials and Fabrication

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

Affiliations

School of Materials and Chemistry

University of Shanghai for Science and Technology

College of Material, Chemistry and Chemical Engineering, Key Laboratory of Organosilicon Chemistry and Material Technology (Ministry of Education)

Hangzhou Normal University

Tianjin Key Laboratory of Chemical Process Safety, Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology

Hebei University of Technology

College of Automotive Engineering

Yancheng Institute of Technology

Funding

Division of Chemical, Bioengineering, Environmental, and Transport Systems · National Natural Science Foundation of China · Higher Education Discipline Innovation Project · National Science Foundation · Hangzhou Normal University · Beijing National Laboratory for Condensed Matter Physics

References (58)

Show source-provided references
1. 10.1021/cr500720t10.1021/cr500720t ↗
2. 10.1002/anie.20160698610.1002/anie.201606986 ↗
3. 10.1039/D2CS00765G10.1039/D2CS00765G ↗
4. 10.1021/acsenergylett.9b0133210.1021/acsenergylett.9b01332 ↗
5. 10.20517/energymater.2023.9110.20517/energymater.2023.91 ↗
6. 10.1038/s41570-022-00394-610.1038/s41570-022-00394-6 ↗
7. 10.1016/j.jpowsour.2020.22880410.1016/j.jpowsour.2020.228804 ↗
8. 10.1002/anie.20160492510.1002/anie.201604925 ↗
9. 10.1016/j.coelec.2021.10083610.1016/j.coelec.2021.100836 ↗
10. 10.1021/acsenergylett.2c0019810.1021/acsenergylett.2c00198 ↗
11. 10.1002/adfm.20231062010.1002/adfm.202310620 ↗
12. 10.1038/nmat480810.1038/nmat4808 ↗
13. 10.1016/j.nanoen.2022.10696310.1016/j.nanoen.2022.106963 ↗
14. 10.1002/adma.20140584010.1002/adma.201405840 ↗
15. 10.1021/acsenergylett.8b0189910.1021/acsenergylett.8b01899 ↗
16. 10.1002/aenm.20140067810.1002/aenm.201400678 ↗
17. 10.1016/j.ensm.2018.06.00810.1016/j.ensm.2018.06.008 ↗
18. 10.1039/c2cs35178a10.1039/c2cs35178a ↗
19. 10.1016/j.elecom.2021.10702810.1016/j.elecom.2021.107028 ↗
20. 10.1021/acs.accounts.0c0036010.1021/acs.accounts.0c00360 ↗
21. 10.1002/chem.20060173810.1002/chem.200601738 ↗
22. 10.1016/j.electacta.2017.12.13110.1016/j.electacta.2017.12.131 ↗
23. 10.1016/j.jpowsour.2018.05.05310.1016/j.jpowsour.2018.05.053 ↗
24. 10.1002/adma.20200856010.1002/adma.202008560 ↗
25. 10.1002/asia.20220090110.1002/asia.202200901 ↗
26. 10.1016/j.electacta.2024.14524210.1016/j.electacta.2024.145242 ↗
27. 10.1002/anie.20210372210.1002/anie.202103722 ↗
28. 10.1016/j.molliq.2023.12360510.1016/j.molliq.2023.123605 ↗
29. 10.1016/j.molliq.2024.12433210.1016/j.molliq.2024.124332 ↗
30. 10.1002/anie.20190243310.1002/anie.201902433 ↗
31. 10.1021/acsomega.3c0229710.1021/acsomega.3c02297 ↗
32. 10.1039/D2SC03450F10.1039/D2SC03450F ↗
33. 10.1039/D0TA07891C10.1039/D0TA07891C ↗
34. 10.1039/C5EE02341F10.1039/C5EE02341F ↗
35. 10.1038/s41467-020-17662-y10.1038/s41467-020-17662-y ↗
36. 10.1039/D2EE03617G10.1039/D2EE03617G ↗
37. 10.1002/adfm.20240531410.1002/adfm.202405314 ↗
38. 10.1016/j.jelechem.2011.10.01510.1016/j.jelechem.2011.10.015 ↗
39. 10.1021/ac60230a01610.1021/ac60230a016 ↗
40. 10.1002/cjoc.1996014041010.1002/cjoc.19960140410 ↗
41. 10.1016/j.chempr.2016.09.00410.1016/j.chempr.2016.09.004 ↗
42. 10.1021/acsnano.0c0128110.1021/acsnano.0c01281 ↗
43. 10.1126/science.124962510.1126/science.1249625 ↗
44. 10.1021/jacs.6b1098410.1021/jacs.6b10984 ↗
45. 10.1016/j.joule.2018.04.00810.1016/j.joule.2018.04.008 ↗
46. 10.1021/jacs.7b0114610.1021/jacs.7b01146 ↗
47. 10.1039/C6EE02057G10.1039/C6EE02057G ↗
48. 10.1002/anie.20140613510.1002/anie.201406135 ↗
49. 10.1002/anie.20170339910.1002/anie.201703399 ↗
50. 10.1002/anie.20150144310.1002/anie.201501443 ↗
51. 10.1039/D2NJ03495F10.1039/D2NJ03495F ↗
52. 10.1016/j.ijheatmasstransfer.2023.12392410.1016/j.ijheatmasstransfer.2023.123924 ↗
53. 10.1021/jacs.1c1354310.1021/jacs.1c13543 ↗
54. 10.1021/acssuschemeng.1c0719010.1021/acssuschemeng.1c07190 ↗
55. 10.1039/C6TA01177B10.1039/C6TA01177B ↗
56. 10.1016/j.jpowsour.2020.22913210.1016/j.jpowsour.2020.229132 ↗
57. 10.1002/anie.20210721610.1002/anie.202107216 ↗
58. 10.1016/j.jechem.2018.09.02010.1016/j.jechem.2018.09.020 ↗