Iron-oxalato framework with one-dimensional open channels for electrochemical sodium-ion intercalation

Abstract

Discovery of a new class of ion intercalation compounds is highly desirable due to its relevance to various electrochemical devices, such as batteries. Herein, we present a new iron-oxalato open framework, which showed reversible Na(+) intercalation/extraction. The hydrothermally synthesized K4Na2[Fe(C2O4)2]3⋅2 H2O possesses one-dimensional open channels in the oxalato-bridged network, providing ion accessibility up to two Na(+) per the formula unit. The detailed studies on the structural and electronic states revealed that the framework exhibited a solid solution state almost entirely during Na(+) intercalation/extraction associated with the reversible redox of Fe. The present work demonstrates possibilities of the oxalato frameworks as tunable and robust ion intercalation electrode materials for various device applications.

Keywords: Mössbauer spectroscopy; electrochemistry; metal-organic frameworks; oxalates; sodium-ion batteries.