Publication date: 10th April 2024
The Thermally Regenerative Electrochemical Cycle (TREC) system utilizes the temperature-dependent potential variations of electrodes. It charges at lower voltages in high temperatures and discharges at higher voltages in low temperatures. This process allows for efficient harvesting of low-grade thermal energy, with significant recent increases in interest in this field. In this study, we performed first-principles calculations to discover how differences in the number of water molecules create variations in bond covalency. These variations lead to changes in the structural vibration modes, which in turn influence the efficiency of TREC systems. From ab initio molecular dynamics simulations at varying temperatures, we discovered that increasing the synthesis temperature leads to a reduction in coordinated water molecules in the Prussian Blue analogs (PBA). This observation is consistent with the trends we've seen in our experimental data. Electronic structure calculations revealed that the presence of water molecules impacts the covalency of bonds around Fe atoms. This alteration is associated with changes in the A1g peak intensity observed in Raman spectroscopy. Our results provide guidelines for research on electrochemical systems that include Prussian Blue analogs (PBA).
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