Solvation Structure of Methanol-in-Salt Electrolyte Revealed by Small-Angle X-ray Scattering and SimulationsClick to copy article linkArticle link copied!
- Xingyi LyuXingyi LyuDepartment of Chemistry and Biochemistry, Northern Illinois University, DeKalb, Illinois 60115, United StatesMore by Xingyi Lyu
- Haimeng WangHaimeng WangMaterials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Haimeng Wang
- Xinyi LiuXinyi LiuDepartment of Chemistry and Biochemistry, Northern Illinois University, DeKalb, Illinois 60115, United StatesMore by Xinyi Liu
- Lilin HeLilin HeNeutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesMore by Lilin He
- Changwoo DoChangwoo DoNeutron Scattering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesMore by Changwoo Do
- Soenke SeifertSoenke SeifertX-ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Soenke Seifert
- Randall E. WinansRandall E. WinansX-ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Randall E. Winans
- Lei Cheng*Lei Cheng*E-mail: [email protected].Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United StatesChemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United StatesMore by Lei Cheng
- Tao Li*Tao Li*E-mail: [email protected]Department of Chemistry and Biochemistry, Northern Illinois University, DeKalb, Illinois 60115, United StatesX-ray Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United StatesMore by Tao Li
Abstract
The solvation structure of water-in-salt electrolytes was thoroughly studied, and two competing structures─anion solvated structure and anion network─were well-defined in recent publications. To further reveal the solvation structure in those highly concentrated electrolytes, particularly the influence of solvent, methanol was chosen as the solvent for this proposed study. In this work, small-angle X-ray scattering, small-angle neutron scattering, Fourier-transform infrared spectroscopy, and Raman spectroscopy were utilized to obtain the global and local structural information. With the concentration increment, the anion network formed by TFSI– became the dominant structure. Meanwhile, the hydrogen bonds among methanol were interrupted by the TFSI– anion and formed a new connection with them. Molecular dynamic simulations with two different force fields (GAFF and OPLS-AA) are tested, and GAFF agreed with synchrotron small-angle X-ray scattering/wide-angle X-ray scattering (SAXS/WAXS) results well and provided insightful information about molecular/ion scale solvation structure. This article not only deepens the understanding of the solvation structure in highly concentrated solutions, but more importantly, it provides additional strong evidence for utilizing SAXS/WAXS to validate molecular dynamics simulations.
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