Unconventional interfacial water structure of highly concentrated aqueous electrolytes at negative electrode polarizations

Chao-Yu Li, Ming Chen, Shuai Liu, Xinyao Lu, Jinhui Meng, Jiawei Yan, Héctor D. Abruña, Guang Feng () and Tianquan Lian ()
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Chao-Yu Li: Emory University
Ming Chen: Huazhong University of Science and Technology (HUST)
Shuai Liu: Xiamen University
Xinyao Lu: Cornell University
Jinhui Meng: Emory University
Jiawei Yan: Xiamen University
Héctor D. Abruña: Cornell University
Guang Feng: Huazhong University of Science and Technology (HUST)
Tianquan Lian: Emory University

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract Water-in-salt electrolytes are an appealing option for future electrochemical energy storage devices due to their safety and low toxicity. However, the physicochemical interactions occurring at the interface between the electrode and the water-in-salt electrolyte are not yet fully understood. Here, via in situ Raman spectroscopy and molecular dynamics simulations, we investigate the electrical double-layer structure occurring at the interface between a water-in-salt electrolyte and an Au(111) electrode. We demonstrate that most interfacial water molecules are bound with lithium ions and have zero, one, or two hydrogen bonds to feature three hydroxyl stretching bands. Moreover, the accumulation of lithium ions on the electrode surface at large negative polarizations reduces the interfacial field to induce an unusual “hydrogen-up” structure of interfacial water and blue shift of the hydroxyl stretching frequencies. These physicochemical behaviours are quantitatively different from aqueous electrolyte solutions with lower concentrations. This atomistic understanding of the double-layer structure provides key insights for designing future aqueous electrolytes for electrochemical energy storage devices.

Date: 2022
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DOI: 10.1038/s41467-022-33129-8

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