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1.
Nat Commun ; 15(1): 2922, 2024 Apr 04.
Article in English | MEDLINE | ID: mdl-38575605

ABSTRACT

Aluminum current collectors are widely used in nonaqueous batteries owing to their cost-effectiveness, lightweightness, and ease of fabrication. However, they are excluded from aqueous batteries due to their severe corrosion in aqueous solutions. Here, we propose hydrolyzation-type anodic additives to form a robust passivation layer to suppress corrosion. These additives dramatically lower the corrosion current density of aluminum by nearly three orders of magnitude to ~10-6 A cm-2. In addition, realizing that electrochemical corrosion accompanies anode prelithiation, we propose a prototype of self-prolonging aqueous Li-ion batteries (Al ||LiMn2O4 ||TiO2), whose capacity retention rises from 49.5% to 70.1% after 200 cycles. A sacrificial aluminum electrode where electrochemical corrosion is utilized is introduced as an electron supplement to prolong the cycling life of aqueous batteries. Our work addresses the short-life issue of aqueous batteries resulting from the corrosion of the current collector and lithium loss from side reactions.

2.
Adv Mater ; 34(47): e2207040, 2022 Nov.
Article in English | MEDLINE | ID: mdl-36121604

ABSTRACT

High-concentration water-in-salt (WIS) electrolytes expand the stable electrochemical window of aqueous electrolytes, leading to the advent of high-voltage (above 2 V) aqueous Li-ion batteries (ALIBs). However, the high lithium salt concentration electrolytes of ALIBs result in their high cost and deteriorate kinetic performance. Therefore, it is challenging for ALIBs to explore aqueous electrolytes with appropriate concentration to balance the electrochemical window and kinetic performance as well as the cost. In contrast to maintaining high concentrations of aqueous electrolytes (>20 m), a small number of hydrophobic cations are introduced to a much lower electrolyte concentration (13.8 m), and it is found that, compared with WIS electrolytes, ALIBs with these concentration-lowered electrolytes possess a compatible stable electrochemical window (3.23 V) and achieve better kinetic performance. These findings originate from the added cations, which form an electric-field-reinforced hydrophobic cationic sieve (HCS) that blocks water away from the anode and suppresses the hydrogen evolution reaction. Meanwhile, the lower electrolyte concentration provides significant benefits to ALIBs, including lower cost, better rate capability (lower viscosity of 18 cP and higher ionic conductivity of 22 mS cm-1 at 25 °C), and improved low-temperature performance (liquidus temperature of -10.18 °C).

3.
Adv Mater ; 32(2): e1904427, 2020 Jan.
Article in English | MEDLINE | ID: mdl-31782981

ABSTRACT

Water-in-salt (WiS) electrolytes provide a new pathway to widen the electrochemical window of aqueous electrolytes. However, their formulation strongly depends on the solubility of the chosen salts, imposing a stringent restriction on the number of possible WiS systems. This issue becomes more severe for aqueous Na-ion batteries (ANIBs) owing to the relatively lower solubility of sodium salts compared to its alkaline cousins (Li, K, and Cs). A new class of the inert-cation-assisted WiS (IC-WiS) electrolytes containing the tetraethylammonium (TEA+ ) inert cation is reported. The Na IC-WiS electrolyte at a superhigh concentration of 31 mol kg-1 exhibits a wide electrochemical window of 3.3 V, suppresses transition metal dissolution from the cathode, and ensures singular intercalation of Na into both cathode and anode electrodes during cycling, which is often problematic in mixed alkali cation systems such as K-Na and Li-Na. Owing to these unique advantages of the IC-WiS electrolyte, the NaTiOPO4 anode and Prussian blue analog Na1.88 Mn[Fe(CN)6 ]0.97 ·1.35H2 O cathode can be coupled to construct a full ANIB, delivering an average voltage of 1.74 V and a high energy density of 71 Wh kg-1 with a capacity retention of 90% after 200 cycles at 0.25C and of 76% over 800 cycles at 1C.

4.
ACS Appl Mater Interfaces ; 11(44): 41356-41362, 2019 Nov 06.
Article in English | MEDLINE | ID: mdl-31603299

ABSTRACT

Prussian blue analogues (PBAs) are considered to be ideal multivalent cation host materials due to their unique open-framework structure. In aqueous solution, however, the PBAs' cathodes have a low reversible capacity limited by the single electrochemical group Fe(CN)63- and high crystal water content. They also suffer from fast cycle fading, resulting from significant oxygen/hydrogen evolution and cathode dissolution. In this work, a high-capacity PBA-type FeFe(CN)6 cathode with double transition metal redox sites is successfully demonstrated in 5 m Al(CF3SO3)3 Water-in-Salt electrolyte (Al-WISE). Due to Al-WISE having a wide electrochemical window (2.65 V) and low dissolution of the cathode, our PBA cathode exhibits a high discharge capacity of 116 mAh/g and the superior cycle stability >100 cycles with capacity fading of 0.39% per cycle.

5.
Materials (Basel) ; 11(2)2018 Feb 23.
Article in English | MEDLINE | ID: mdl-29473881

ABSTRACT

In this work, a three dimensional (3D) graphene-nitrogen doped carbon nanotubes (G-NCNTs) network was successfully fabricated on the surface of a glassy carbon (GC) electrode using the pulse potential method (PPM) in a graphene oxide-nitrogen doped carbon nanotubes (GO-NCNTs) dispersion. The morphological and characteristics of GO-NCNTs and G-NCNTs nanocomposites were investigated by atomic force microscopy (AFM), scanning electron microscopy (SEM), UV-vis spectroscopy, Raman spectroscopy, and electrochemical experiments. The 3DG-NCNTs network was applied as a new voltammetric material for the fabrication of an electrochemical platform for determination of urapidil. Systematic electrochemical tests demonstrate that the 3DG-NCNTs network modified GC electrode can effectively increase the response to the oxidation of urapidil. Under the optimum conditions, the electrochemical response was linear with urapidil concentrations in the range of 1.0 × 10-8~2.0 × 10-6 mol·L-1, while a low detection limit of 5.0 × 10-9 mol·L-1 was obtained for urapidil. Moreover, the proposed sensing platform exhibited good results for sensitivity, reproducibility, selectivity, and stability, which makes it very suitable for use as an ideal inexpensive and rapid analytical method applicable for complex drug matrices.

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