Correlation of electrochemical and ab initio investigations of iron poly-bipyridine coordination complexes for battery applications: impact of the anionic environment and the local geometries of the redox complexes on the electrochemical response
文献情報
Adama Sy, Asif Iqbal Bhatti, Fahim Hamidouche, Olivier Le Bacq, Lauréline Lecarme, Jean-Claude Leprêtre
Although they exhibit huge versatility, coordination complexes have been rarely investigated in the field of cathode materials for batteries. Despite their relatively high molecular mass, according to the nature of the metallic center and that of the ligand, the E° value and the electron transfer kinetics can be adjusted to develop a performant material compatible with the electrolyte. Here, we propose to investigate FeII poly-bipyridine complexes with a view to check the impact of the nature of the electrolyte as well as the influence of the distance between two redox centers when polymerized on the electrochemical response in battery conditions. To understand these changes, three lithium salts have been studied: LiClO4, LiPF6 and LiTFSI (TFSI = bis(trifluoromethane)sulfonimide). In order to mimic these impacts, monomer complexes (mono- and binuclear) have been electrochemically studied, whereas, thanks to ab initio calculations, their redox behavior has been correlated to the ligand environment of the metallic center. Finally, despite their expected low mass capacity, these polymeric coordination complexes have been involved in battery conditions.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.













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