AUTHOR=Willenberg Shane , Carleschi Emanuela , Ross Natasha TITLE=Spectroscopic and Electrochemical Exploration of Carbon-Infused Intercalation-Type Spinel Composite for Aqueous Systems JOURNAL=Frontiers in Chemistry VOLUME=Volume 10 - 2022 YEAR=2022 URL=https://www.frontiersin.org/journals/chemistry/articles/10.3389/fchem.2022.890291 DOI=10.3389/fchem.2022.890291 ISSN=2296-2646 ABSTRACT=Lithium manganese based compounds are promising intercalation host materials for aqueous battery systems due to their synergy with high ionic conductive aqueous electrolyte, safety, eco-friendliness, as well as low cost. Yet, due to poor electrical conductivity and trapping of diffused electrolyte cations within its crystal formation, achieving optimum cycle stability and rate capability remains a challenge. Alas, limiting their use in modern day high-powered devices which require quality output with high reliability. Here, the authors propose a facile method to produce LiMn2O4 and LiFe0.5Mn0.5PO4 and compare their structural stability and corresponding electrochemical performance by controlling the interfacial layer through multi-walled carbon nanotubes (MWCNTs) infusion. High resolution scanning electron microscopy results revealed that the active particles were connected by MWCNT via the formation of a three-dimensional wiring network, suggesting that stronger interfacial bonding exists within the composite. As a result, the conducting composite decreases the electron transport distance with increased number of active sites thus accelerating the lithium ion intercalation/de-intercalation process. Compared to C/LMO with a Rct of 226.3 Ohm and change transfer (io) of 2.75 x10-3, the C/LFMPO-composite has a reduced Rct of 138 Ohm and enhanced rate of 1.86 x 10-4 A cm-2 . The faster kinetics can be attributed to the unique synergy between the conductive MWCNTs and the contribution of both single-phase and two-phase regions in Li1-x(Fe,Mn)PO4 during Li+ extraction and insertion. The electrochemical features before and after modification correlate well with the interplanar distance of the expanded manganese and manganese phosphate layers shown by their unique surface features, as analysed by advanced spectroscopy techniques. The results reveal that MWCNTs facilitates faster electron transmission whilst maintaining the stability of the host framework which proves favorable as next generation cathode materials.