Solvation Structure Regulation for Highly Reversible Aqueous Al Metal Batteries

Zhao, Zhongchen; Zhang, Zonghan; Xu, Tian; Wang, Wenbin; Wang, Baofeng; Yu, Xuebin

doi:10.1021/jacs.3c13003

Cited by 10 publications

(4 citation statements)

References 41 publications

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“…In contrast, uniform and dense deposition without obvious corrosion occurs on the surface of the Al electrode in the AATH40 electrolyte (Figure d). In addition, to test the suitability of the electrolyte, a titanium (Ti) sheet was used as the substrate for depositing Al . Real-time images were captured at the electrode/electrolyte interface by using an optical microscope.…”

Section: Resultsmentioning

confidence: 99%

Air-Stable and Low-Cost High-Voltage Hydrated Eutectic Electrolyte for High-Performance Aqueous Aluminum-Ion Rechargeable Battery with Wide-Temperature Range

Luo,

Wang,

Zhang

et al. 2024

ACS Nano

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Aqueous aluminum-ion batteries (AAIBs) are considered as a promising alternative to lithium-ion batteries due to their large theoretical capacity, high safety, and low cost. However, the uneven deposition, hydrogen evolution reaction (HER), and corrosion during cycling impede the development of AAIBs, especially under a harsh environment. Here, a hydrated eutectic electrolyte (AATH40) composed of Al(OTf) 3 , acetonitrile (AN), triethyl phosphate (TEP), and H 2 O was designed to improve the electrochemical performance of AAIBs in a wide temperature range. The combination of molecular dynamics simulations and spectroscopy analysis reveals that AATH40 has a less-water-solvated structure [Al(AN) 2 (TEP)(OTf) 2 (H 2 O)] 3+ , which effectively inhibits side reactions, decreases the freezing point, and extends the electrochemical window of the electrolyte. Furthermore, the formation of a solid electrolyte interface, which effectively inhibits HER and corrosion, has been demonstrated by X-ray photoelectron spectroscopy, X-ray diffraction tests, and in situ differential electrochemical mass spectrometry. Additionally, operando synchrotron Fourier transform infrared spectroscopy and electrochemical quartz crystal microbalance with dissipation monitoring reveal a three-electron storage mechanism for the Al//polyaniline full cells. Consequently, AAIBs with this electrolyte exhibit improved cycling stability within the temperature range of −10−50 °C. This present study introduces a promising methodology for designing electrolytes suitable for low-cost, safe, and stable AAIBs over a wide temperature range.

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Section: Resultsmentioning

confidence: 99%

Air-Stable and Low-Cost High-Voltage Hydrated Eutectic Electrolyte for High-Performance Aqueous Aluminum-Ion Rechargeable Battery with Wide-Temperature Range

Luo,

Wang,

Zhang

et al. 2024

ACS Nano

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“…The cells can typically work under bending, rolling, or puncturing treatment . Furthermore, the Yu group at Fudan University reported that water activity in the electrolyte can be suppressed by optimizing the Al 3+ solvation structure through intercalation of polar pyridine-3-carboxylic acid in an aluminum trifluoromethanesulfonate aqueous environment. The Al corrosion in the hybrid electrolyte was restrained, and the long-term electrochemical stability of the electrolyte was tremendously improved.…”

Section: Discussionmentioning

confidence: 99%

Unveiling the Reaction Mechanism of Aluminum and Its Alloy Anode in Aqueous Aluminum Cells

Wu,

Lin,

Tsai

et al. 2024

ACS Appl. Energy Mater.

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Aqueous aluminum-ion batteries (AAIBs) are attractive electrochemical cells for energy storage because of Earth's crust abundance, inexpensiveness, high theoretical capacity, and safety of aluminum. However, state-of-the-art AAIBs based on aluminum or its alloy anode show ambiguity in the detailed charge−discharge reactions, and the activation mechanisms still need to be explored. Herein, we investigate the effects of surface modification (treated aluminum in ionic liquids (T-Al)) or the alloying approach (Al−Cu alloy or Zn−Al alloy) in different anionic aqueous aluminum-based electrolytes (e.g., 1 M Al(OTF) 3 , AlCl 3 , and Al(NO 3 ) 3 ). Neither the surface modification nor the alloying approach can support the rechargeability of aluminum atoms from the employed aqueous electrolytes. During the charge−discharge cycles of the symmetric cells in the aqueous electrolytes, the dissolution of aluminum and its alloy, accompanied by severe gas evolution, was observed. These corrosion reactions resulted in corrosive activity of aluminum and its alloy in these selected aqueous electrolytes. The aluminum and T-Al anode activity in these aqueous electrolytes was mainly induced by the chloride anions present in the aqueous electrolytes or residual in the treated artificial solid−electrolyte interface layer. For the activity of the Al−Cu alloy, nanolamellar Al 2 Cu served as the catalyst and kept the hydrolysis by α-Al in aqueous electrolytes to continuously generate H 2 . The Zn−Al alloy anode exhibited a severe gas evolution reaction in these aqueous electrolytes and, therefore, showed the highest activity among these Al anodes. Thus, for the first time, the present work clarified the mechanisms of reactions occurring at the Al anode using the surface modification or alloying approach of aqueous electrolyte Al cells.

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“…Aluminium is the most abundant metal on earth, with a low redox potential (−1.67 V vs. SHE), high volumetric capacity (8056 mA h cm −3 ), low cost, and safety in aqueous solutions. 149 Therefore, AABs have received increasing attention. However, the low activity of the air electrode and the formation of by-products, Al oxide/hydroxide or hydrogen, lead to a low practical specific energy of ∼1000 W h kg −1 .…”

Section: Flexible Metal–air Batteriesmentioning

confidence: 99%

Flexible electrochemical energy storage devices and related applications: recent progress and challenges

Xiao,

et al. 2024

Chem. Sci.

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Solvation Structure Regulation for Highly Reversible Aqueous Al Metal Batteries

Cited by 10 publications

References 41 publications

Air-Stable and Low-Cost High-Voltage Hydrated Eutectic Electrolyte for High-Performance Aqueous Aluminum-Ion Rechargeable Battery with Wide-Temperature Range

Air-Stable and Low-Cost High-Voltage Hydrated Eutectic Electrolyte for High-Performance Aqueous Aluminum-Ion Rechargeable Battery with Wide-Temperature Range

Unveiling the Reaction Mechanism of Aluminum and Its Alloy Anode in Aqueous Aluminum Cells

Flexible electrochemical energy storage devices and related applications: recent progress and challenges

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