Benzonitrile-driven discharge of potassium-intercalated carbon allotropes

Steiger F, Edelthalhammer K, Lucherelli MA, Wabra I, Requena-Ramírez J, Castro E, Hauke F, Echegoyen L, Hirsch A, Abellán G, Perez-Ojeda Rodriguez ME (2025)

Publication Type: Journal article

Publication year: 2025

Journal

Pages Range: 120379

Article Number: 120379

DOI: 10.1016/j.carbon.2025.120379

Abstract

In this work we performed a comprehensive investigation, exploring the reduction of synthetic carbon allotropes (SCAs) via alkali metal intercalation. Carbon nanotubes (CNTs), carbon nano-onions (CNOs), and fullerenes (C60&C70) were employed, focusing on post-intercalation electron transfer efficiency and mass transport dynamics with benzonitrile (PhCN). Our study revealed the feasibility of discharging residual negative charges in all allotropes, exhibiting different electron transfer ratios (ETR) dependent on morphological factors. Notably, CNT length played a crucial role, shorter HiPco nanotubes displayed a significantly higher ETR (55 %) compared to longer arc discharge nanotubes (15 %), highlighting the influence of nanotube length on intercalation kinetics. Further investigation into CNOs unveiled a relatively high ETR of 80 % for untreated CNOs and a low ratio of 24 % for oxidized onions, underlining the critical role of size distribution and surface chemistry. Inner shell entrapment of potassium reduces accessibility in CNOs, as confirmed by TGA-MS and XPS experiments. Our analysis underscored the impact of disparate electron affinities and molecular structures on electron transfer dynamics, as seen in our fulleride analysis, where reversible electron uptake from fullerides to solvent occurred, more pronounced for C60 than C70. Overall, our findings demonstrated that CNTs and CNOs share similar mechanisms with graphenides, however, mass transport is limited by potassium accessibility. In contrast, molecular fullerenes exhibit distinct behavior due to competitive redox processes. Additionally, our investigation highlighted the utility of PhCN treatment in facilitating the recovery of pristine materials and mitigating undesired side functionalization post-exposure to moisture, thereby enabling the protocol's generalization across various SCAs.

Authors with CRIS profile

Involved external institutions

The University of Texas at El Paso United States (USA) (US) University of València / Universitat de València Spain (ES)

How to cite

APA:

Steiger, F., Edelthalhammer, K., Lucherelli, M.A., Wabra, I., Requena-Ramírez, J., Castro, E.,... Perez-Ojeda Rodriguez, M.E. (2025). Benzonitrile-driven discharge of potassium-intercalated carbon allotropes. Carbon, 120379. https://doi.org/10.1016/j.carbon.2025.120379

MLA:

Steiger, Florian, et al. "Benzonitrile-driven discharge of potassium-intercalated carbon allotropes." Carbon (2025): 120379.

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