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1.
Nat Commun ; 15(1): 1133, 2024 Feb 07.
Article in English | MEDLINE | ID: mdl-38326356

ABSTRACT

In recent decades, more than 100,000 scientific articles have been devoted to the development of electrode materials for supercapacitors and batteries. However, there is still intense debate surrounding the criteria for determining the electrochemical behavior involved in Faradaic reactions, as the issue is often complicated by the electrochemical signals produced by various electrode materials and their different physicochemical properties. The difficulty lies in the inability to determine which electrode type (battery vs. pseudocapacitor) these materials belong to via simple binary classification. To overcome this difficulty, we apply supervised machine learning for image classification to electrochemical shape analysis (over 5500 Cyclic Voltammetry curves and 2900 Galvanostatic Charge-Discharge curves), with the predicted confidence percentage reflecting the shape trend of the curve and thus defined as a manufacturer. It's called "capacitive tendency". This predictor not only transcends the limitations of human-based classification but also provides statistical trends regarding electrochemical behavior. Of note, and of particular importance to the electrochemical energy storage community, which publishes over a hundred articles per week, we have created an online tool to easily categorize their data.

2.
Small ; 20(4): e2303945, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37705137

ABSTRACT

A water-in-salt electrolyte is a highly concentrated aqueous solution (i.e., 21 mol LiTFSI in 1 kg H2 O) that reduces the number of water molecules surrounding salt ions, thereby decreasing the water activity responsible for decomposition. This electrolyte widens the electrochemical stability window via the formation of a solid electrolyte interphase (SEI) at the electrode surface. However, using high concentration electrolytes in Li-ion battery technology to enhance energy density and increase cycling stability remains challenging. A parasitic reaction, called the hydrogen evolution reaction, occurs when the reaction operates at a lower voltage. It is demonstrated here that a micrometric white layer is indeed a component of the SEI layer, not just on the nanoscale, through the utilization of an operando high-resolution optical microscope. The results indicate that LiTFSI precipitation is the primary species present in the SEI layer. Furthermore, the passivation layer is found to be dynamic since it dissolves back into the electrolyte during open circuit voltage.

3.
J Chem Phys ; 159(10)2023 Sep 14.
Article in English | MEDLINE | ID: mdl-37702360

ABSTRACT

Superconcentrated aqueous electrolytes have recently emerged as a new class of electrolytes, called water-in-salt electrolytes. They are distinguished, in both weight and volume, by a quantity of salt greater than water. Currently, these electrolytes are attracting major interest, particularly for application in aqueous rechargeable batteries. These electrolytes have only a small amount of free water due to an ultrahigh salt concentration. Consequently, the electrochemical stability window of water is wider than the predicted thermodynamic value of 1.23 V. Hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) have been shown to be shifted to more negative and positive potentials, respectively. The decrease in free water population is recognized as being involved in the increase in the electrochemical stability window of water. Here, we study the quantitative contribution of the decrease in the free water molecule concentration to the permittivity of the solution and of the activity of water to the OER and HER overpotentials when the salt concentration increases. We compare our model with that of Kornyshev and get three types of electrolyte structures: diluted, gradient of water contents, and aggregation. The theoretical calculation of the redox potentials of the OER and HER is compared with the experimentally determined electrochemical properties of aqueous LiTFSI electrolytes.

4.
Chem Sci ; 14(23): 6383-6392, 2023 Jun 14.
Article in English | MEDLINE | ID: mdl-37325136

ABSTRACT

The essence of any electrochemical system is engraved in its electrical double layer (EDL), and we report its unprecedented reorganization by the structural isomerism of molecules, with a direct consequence on their energy storage capability. Electrochemical and spectroscopic analyses in combination with computational and modelling studies demonstrate that an attractive field-effect due to the molecule's structural-isomerism, in contrast to a repulsive field-effect, spatially screens the ion-ion coulombic repulsions in the EDL and reconfigures the local density of anions. In a laboratory-level prototype supercapacitor, those with ß-structural isomerism exhibit nearly 6-times elevated energy storage compared to the state-of-the-art electrodes, by delivering ∼535 F g-1 at 1 A g-1 while maintaining high performance metrics even at a rate as high as 50 A g-1. The elucidation of the decisive role of structural isomerism in reconfiguring the electrified interface represents a major step forward in understanding the electrodics of molecular platforms.

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