DataVXACS Applied Materials & InterfacesPaper
journal article·2021-11-10Open access

Enabling Magnesium Anodes by Tuning the Electrode/Electrolyte Interfacial Structure

Xiaoyu Wen, Zhou Yu, Yifan Zhao, Jian Zhang, Rui Qiao, Lei Cheng, Chunmei Ban, Juchen Guo

ACS Applied Materials & Interfaces· Volume 13· Issue 44
Publisher pageOpen full text
Source abstract

Abstract

A new deposition mechanism is presented in this study to achieve highly reversible plating and stripping of magnesium (Mg) anodes for Mg-ion batteries. It is known that the reduction of electrolyte anions such as bis(trifluoromethanesulfonyl)imide (TFSI–) causes Mg surface passivation, resulting in poor electrochemical performance for Mg-ion batteries. We reveal that the addition of sodium cations (Na+) in Mg-ion electrolytes can fundamentally alter the interfacial chemistry and structure at the Mg anode surface. The molecular dynamics simulation suggests that Na+ cations contribute to a significant population in the interfacial double layer so that TFSI– anions are excluded from the immediate interface adjacent to the Mg anode. As a result, the TFSI– decomposition is largely suppressed so does the formation of passivation layers at the Mg surface. This mechanism is supported by our electrochemical, microscopic, and spectroscopic analyses. The resultant Mg deposition demonstrates smooth surface morphology and lowered overpotential compared to the pure Mg(TFSI)2 electrolyte.
Source: openalex_inverted_index · Quality: baseline

Research context

Energy storageMaterials processing

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

Department of Chemical and Environmental Engineering, University of California, Riverside, California 92521, United States

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

Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States

Materials Science and Engineering Program, University of California, Riverside, California 92521, United States

Department of Mechanical Engineering, Virginia Tech, Blacksburg, Virginia 24061, United States

Paul M. Rady Department of Mechanical Engineering, University of Colorado Boulder, Boulder, Colorado 80309, United States

Funding

Division of Chemistry · U.S. Department of Energy · National Science Foundation · Division of Materials Research · Joint Center for Energy Storage Research (JCESR)

References (49)

Show source-provided references
1. 10.1016/j.joule.2018.10.02810.1016/j.joule.2018.10.028 ↗
2. 10.1039/D0NH00379D10.1039/D0NH00379D ↗
3. 10.1149/1.208655310.1149/1.2086553 ↗
4. 10.1021/acs.langmuir.7b0160910.1021/acs.langmuir.7b01609 ↗
5. 10.1039/C5QI00171D10.1039/C5QI00171D ↗
6. 10.1039/C7CC01570D10.1039/C7CC01570D ↗
7. 10.1038/s41560-020-00734-010.1038/s41560-020-00734-0 ↗
8. 10.1021/acsami.9b0003710.1021/acsami.9b00037 ↗
9. Tutusaus O. · Am. Ethnol. · 2015 · 127 · 8011
10. 10.1021/acsenergylett.8b0106110.1021/acsenergylett.8b01061 ↗
11. 10.1002/aenm.20160205510.1002/aenm.201602055 ↗
12. 10.1021/acsami.0c0994810.1021/acsami.0c09948 ↗
13. 10.1021/jacs.5b0100410.1021/jacs.5b01004 ↗
14. 10.1149/2.0161513jes10.1149/2.0161513jes ↗
15. 10.1038/s41557-018-0019-610.1038/s41557-018-0019-6 ↗
16. 10.1021/jp502354h10.1021/jp502354h ↗
17. 10.1021/acs.jpcc.8b0557310.1021/acs.jpcc.8b05573 ↗
18. 10.1080/0149639070120641310.1080/01496390701206413 ↗
19. 10.1021/acs.chemmater.5b0353110.1021/acs.chemmater.5b03531 ↗
20. 10.1016/j.ensm.2019.10.00410.1016/j.ensm.2019.10.004 ↗
21. 10.1038/s42004-019-0186-410.1038/s42004-019-0186-4 ↗
22. 10.1038/srep0313010.1038/srep03130 ↗
23. 10.1002/anie.20120491310.1002/anie.201204913 ↗
24. 10.1021/am507375t10.1021/am507375t ↗
25. Tutusaus, O.; Mohtadi, R. Paving the way towards highly stable and practical electrolytes for rechargeable magnesium batteries. 2015.10.1002/celc.201402207 ↗
26. Wang H. · ACS Energy Lett. · 2019 · 5 · 20010.1021/acsenergylett.9b02211 ↗
27. 10.1021/ct700301q10.1021/ct700301q ↗
28. 10.1063/1.32869310.1063/1.328693 ↗
29. 10.1080/0026897830010285110.1080/00268978300102851 ↗
30. 10.1021/ja962176010.1021/ja9621760 ↗
31. 10.1021/acs.jctc.7b0052010.1021/acs.jctc.7b00520 ↗
32. 10.1021/ja00124a00210.1021/ja00124a002 ↗
33. 10.1021/acsami.8b1038710.1021/acsami.8b10387 ↗
34. 10.1063/1.512139210.1063/1.5121392 ↗
35. 10.1063/1.240842010.1063/1.2408420 ↗
36. 10.1063/1.47959510.1063/1.479595 ↗
37. 10.1002/jcc.1018910.1002/jcc.10189 ↗
38. Frisch, M.; Trucks, G.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Scalmani, G.; Barone, V.; Mennucci, B.; Petersson, G. Gaussian 09, Revision d. 01; Gaussian Inc.: Wallingford, CT, 2009; pp 201.
39. 10.1149/2.0721711jes10.1149/2.0721711jes ↗
40. 10.1021/acsenergylett.7b0077910.1021/acsenergylett.7b00779 ↗
41. 10.1038/3503755310.1038/35037553 ↗
42. 10.1038/nmat431810.1038/nmat4318 ↗
43. 10.1021/acs.langmuir.6b0052310.1021/acs.langmuir.6b00523 ↗
44. 10.1103/PhysRevB.11.60010.1103/PhysRevB.11.600 ↗
45. 10.1016/S0042-207X(99)00121-910.1016/S0042-207X(99)00121-9 ↗
46. 10.1021/acsami.8b0242510.1021/acsami.8b02425 ↗
47. 10.1021/ja00784a01810.1021/ja00784a018 ↗
48. 10.1149/2.1471809jes10.1149/2.1471809jes ↗
49. 10.1021/acsami.8b1519910.1021/acsami.8b15199 ↗