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Application of murexide as a capping agent for fabrication of magnetite anodes for supercapacitors: experimental and first-principle studies

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Abstract

In this study, we investigate the effectiveness of murexide for surface modification of \(\textrm{Fe}_{3}\textrm{O}_{4}\) nanoparticles to enhance the performance of multiwalled carbon nanotube-\(\textrm{Fe}_{3}\textrm{O}_{4}\) supercapacitor anodes. Our experimental results demonstrate significant improvements in electrode performance when murexide is used as a capping or dispersing agent compared to the case with no additives. When murexide is used as a capping agent, we report a capacitance of 4.2 F cm\(^{-2}\) from cyclic voltammetry analysis with good capacitance retention at high scan rates. From impedance measurements, we reveal a substantial decrease in the real part of impedance for samples prepared with murexide, indicating easier charge transfer at more negative electrode potentials, and reinforcing the role of murexide as a capping agent and charge transfer mediator. Density functional theory is used to investigate interactions between the murexide adsorbate and the \(\textrm{Fe}_{3}\textrm{O}_{4}\) (001) surface, with a specific emphasis on adsorption strength, charge transfer, and electronic properties. This theoretical investigation uncovers a strong adsorption enthalpy of − 4.5 eV and allows us to identify the nature of chemical bonds between murexide and the surface, with significant charge transfer taking place between the \(\textrm{Fe}_{3}\textrm{O}_{4}\) surface and murexide adsorbate. The transfer of electrons from the \(\textrm{Fe}_{3}\textrm{O}_{4}\) surface to murexide is recognized as a vital component of the adsorption process. By examining the bonding nature of murexide on \(\textrm{Fe}_{3}\textrm{O}_{4}\), this research study uncovers insights and proposes a novel bonding configuration of murexide that incorporates a combination of bridging and chelating bonding.

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Data availibility

The raw data (VASP input and structure files) required to reproduce computational findings are available in the Zenodo file repository [48].

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Acknowledgements

This research was funded by the Natural Sciences and Engineering Research Council of Canada, grant number RGPIN-2018-04014, and Faculty of Engineering of McMaster University. Calculations were performed using the Compute Canada infrastructure supported by the Canada Foundation for Innovation under John R. Evans Leaders Fund.

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Authors and Affiliations

  1. Department of Materials Science and Engineering, McMaster University, 1280 Main Street West, Hamilton, ON, 100190, Canada

    Coulton Boucher, Dalue Tang, Igor Zhitomirsky & Oleg Rubel

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Contributions

Conceptualization was prepared by I.Z. and C.B.; carrying out experiments and calculations and writing original draft were done by C.B. and D.T.; data analysis and interpretation were revised by C.B., D.T., I.Z., and O.R.; manuscript review and editing were analyzed by I.Z. and O.R.

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Correspondence to Oleg Rubel.

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Boucher, C., Tang, D., Zhitomirsky, I. et al. Application of murexide as a capping agent for fabrication of magnetite anodes for supercapacitors: experimental and first-principle studies. J Mater Sci 59, 5480–5497 (2024). https://doi.org/10.1007/s10853-024-09524-5

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