Operando 红外光谱监测 Ti3C2TX MXene 中盐包水电解质的氢键重组,The Journal of Physical Chemistry Letters

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Operando 红外光谱监测 Ti3C2TX MXene 中盐包水电解质的氢键重组
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2023-02-07 , DOI: 10.1021/acs.jpclett.2c03769
Mailis Lounasvuori ₁ , Tyler S Mathis ₂ , Yury Gogotsi ₂ , Tristan Petit ₁

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与传统的稀释水性电解质相比，高浓度的盐包水水性电解质具有更宽的电势窗口。结合 MXenes，一种二维过渡金属碳化物和氮化物系列，具有令人印象深刻的电荷存储能力，盐包水电解质是替代电化学储能设备中易燃和有毒有机溶剂的潜在候选者。最近在锂基水盐电解质中Ti ₃ C ₂ T _x MXene 电极的电化学循环过程中发现了一种新的电荷存储机制，这归因于溶剂化 Li ⁺离子在阳极电位下的嵌入和脱嵌。^{然而，Li +}状态的直接证据循环过程中的溶剂化仍然缺失。在这里，我们使用原位红外光谱研究了在盐包水电解质中的电化学循环过程中插入 MXene 层之间的水的氢键键合。发现受限水的氢键状态随着电位和层间空间中Li ^{+离子浓度的变化而显着变化。}这项研究从根本上提供了对电解质结构变化的新见解，同时在 MXene 夹层空间中嵌入 Li ^{+ 。}

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Hydrogen-Bond Restructuring of Water-in-Salt Electrolyte Confined in Ti3C2Tx MXene Monitored by Operando Infrared Spectroscopy

Highly concentrated water-in-salt aqueous electrolytes exhibit a wider potential window compared to conventional, dilute aqueous electrolytes. Coupled with MXenes, a family of two-dimensional transition metal carbides and nitrides with impressive charge storage capabilities, water-in-salt electrolytes present a potential candidate to replace flammable and toxic organic solvents in electrochemical energy storage devices. A new charge storage mechanism was recently discovered during electrochemical cycling of Ti₃C₂T_x MXene electrodes in lithium-based water-in-salt electrolytes, attributed to intercalation and deintercalation of solvated Li⁺ ions at anodic potentials. Nevertheless, direct evidence of the state of Li⁺ solvation during cycling is still missing. Here, we investigate the hydrogen bonding of water intercalated between MXene layers during electrochemical cycling in a water-in-salt electrolyte with operando infrared spectroscopy. The hydrogen-bonding state of the confined water was found to change significantly as a function of potential and the concentration of Li⁺ ions in the interlayer space. This study provides fundamentally new insights into the electrolyte structural changes while intercalating Li⁺ in the MXene interlayer space.

更新日期：2023-02-07

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