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

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,...

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Published inNature communications Vol. 13; no. 1; p. 5330
Main Authors Li, Chao-Yu, Chen, Ming, Liu, Shuai, Lu, Xinyao, Meng, Jinhui, Yan, Jiawei, Abruña, Héctor D., Feng, Guang, Lian, Tianquan
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 10.09.2022
Nature Publishing Group
Nature Portfolio
Subjects
140/133
142/136
639/301/299/161
639/301/299/161/891
639/301/930/12
639/638/542
639/638/630
Aqueous electrolytes
Blue shift
Dynamic structural analysis
Electrochemistry
Electrodes
Electrolytes
Energy storage
Humanities and Social Sciences
Hydrogen bonding
Hydrogen bonds
Ions
Lithium
Lithium ions
Molecular dynamics
multidisciplinary
Raman spectroscopy
Salts
Science
Science (multidisciplinary)
Storage systems
Stretching
Toxicity
Water chemistry
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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. Water-in-salt electrolytes can be useful for future electrochemical energy storage systems. Here, the authors investigate the potential-dependent double-layer structures at the interface between a gold electrode and a highly concentrated aqueous electrolyte solution via in situ Raman measurements.
AbstractList Water-in-salt electrolytes can be useful for future electrochemical energy storage systems. Here, the authors investigate the potential-dependent double-layer structures at the interface between a gold electrode and a highly concentrated aqueous electrolyte solution via in situ Raman measurements.
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. Water-in-salt electrolytes can be useful for future electrochemical energy storage systems. Here, the authors investigate the potential-dependent double-layer structures at the interface between a gold electrode and a highly concentrated aqueous electrolyte solution via in situ Raman measurements.
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.
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.Water-in-salt electrolytes can be useful for future electrochemical energy storage systems. Here, the authors investigate the potential-dependent double-layer structures at the interface between a gold electrode and a highly concentrated aqueous electrolyte solution via in situ Raman measurements.
ArticleNumber 5330
Author Lian, Tianquan
Chen, Ming
Lu, Xinyao
Liu, Shuai
Li, Chao-Yu
Yan, Jiawei
Abruña, Héctor D.
Meng, Jinhui
Feng, Guang
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  orcidid: 0000-0002-2188-5472
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  organization: State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology (HUST)
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  surname: Liu
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  fullname: Abruña, Héctor D.
  organization: Department of Chemistry and Chemical Biology, Cornell University
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  orcidid: 0000-0001-6659-9181
  surname: Feng
  fullname: Feng, Guang
  email: gfeng@hust.edu.cn
  organization: State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology (HUST)
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SSID ssj0000391844
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Snippet Water-in-salt electrolytes are an appealing option for future electrochemical energy storage devices due to their safety and low toxicity. However, the...
Abstract Water-in-salt electrolytes are an appealing option for future electrochemical energy storage devices due to their safety and low toxicity. However,...
Water-in-salt electrolytes can be useful for future electrochemical energy storage systems. Here, the authors investigate the potential-dependent double-layer...
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StartPage 5330
SubjectTerms 140/133
142/136
639/301/299/161
639/301/299/161/891
639/301/930/12
639/638/542
639/638/630
Aqueous electrolytes
Blue shift
Dynamic structural analysis
Electrochemistry
Electrodes
Electrolytes
Energy storage
Humanities and Social Sciences
Hydrogen bonding
Hydrogen bonds
Ions
Lithium
Lithium ions
Molecular dynamics
multidisciplinary
Raman spectroscopy
Salts
Science
Science (multidisciplinary)
Storage systems
Stretching
Toxicity
Water chemistry
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Title Unconventional interfacial water structure of highly concentrated aqueous electrolytes at negative electrode polarizations
URI https://link.springer.com/article/10.1038/s41467-022-33129-8
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https://pubmed.ncbi.nlm.nih.gov/PMC9464189
https://doaj.org/article/236d84d6186043dabc1baa551dd0f25f
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