Abstract
Organic materials are receiving an increasing amount of attention as electrode materials for future post lithium-ion batteries due to their versatility and sustainability. However, their electrochemical reaction mechanism has seldom been investigated. This is a direct consequence of a lack of straightforward and broadly available analytical techniques. Herein, a straightforward in operando attenuated total reflectance infrared spectroscopy method is developed that allows visualization of changes of all infrared active bands that occur as a consequence of reduction/oxidation processes. In operando infrared spectroscopy is applied to the analysis of three different organic polymer materials in lithium batteries. Moreover, this in operando method is further extended to investigation of redox reaction mechanism of poly(anthraquinonyl sulfide) in a magnesium battery, where a reduction of carbonyl bond is demonstrated as a mechanism of electrochemical activity. Conclusions done by the in operando results are complemented by synthesis of model compound and density functional theory calculation of infrared spectra.
Highlights
Organic materials are receiving an increasing amount of attention as electrode materials for future post lithium-ion batteries due to their versatility and sustainability
We show in operando measurements based on attenuated total reflectance (ATR)-IR of the electrode composite inside a modified pouch cell on the established redox-active polymer, poly(anthraquinonyl sulfide) (PAQS), that has been used in several battery systems (Li, Na, Mg, K)[8,14,16,23]
To confirm the applicability of our in operando ATR-IR method to other compounds, we have extended our study to polyanthraquinone (PAQ) and polyaniline (PANI) electroactive compounds
Summary
Organic materials are receiving an increasing amount of attention as electrode materials for future post lithium-ion batteries due to their versatility and sustainability Their electrochemical reaction mechanism has seldom been investigated. In operando infrared spectroscopy is applied to the analysis of three different organic polymer materials in lithium batteries This in operando method is further extended to investigation of redox reaction mechanism of poly (anthraquinonyl sulfide) in a magnesium battery, where a reduction of carbonyl bond is demonstrated as a mechanism of electrochemical activity. The electrochemical reaction mechanism inside of organic battery cathodes have been investigated by X-ray diffraction[17], nuclear magnetic resonance (NMR)[18], Raman and infrared (IR) spectroscopy[17,19,20]. Interpretation of experimental ATR-IR spectra is supported by quantum mechanical calculation based on density functional theory (DFT), which allowed us assignation of bands
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