Exploring the effect of graphite-coating on hexanary high entropy metal oxides towards efficient water electrocatalysis
Abstract
High-entropy oxides (HEOs) have emerged as promising electrocatalysts due to their high configurational entropy, modular electronic structures, and defect-rich multicationic lattices. However, modifying their electrochemical kinetics through conductive surface modification remains completely unknown. An Al-rich hexanary spinel, Cr, Cd, Fe, Mg, and Mn-based materials were synthesized using a sol-gel method and then modified with graphite (5–20 wt%) via rotary ball milling to improve conductivity and interfacial charge transfer, resulting in a stable spinel phase as validated by Rietveld-refined XRD. The addition of graphite significantly increased anodic activity, with the 10 wt% composite (HEO-10C) achieving a peak current density of 47.09 mA cm−2 in 1 M KOH + methanol. This was followed by decreased charge-transfer resistance and better electron-transfer kinetics. The graphite-HEO interface allows for faster reaction pathways, as evidenced by a high diffusion coefficient (8.65 × 10−8 cm2 s−1), a heterogeneous electron-transfer rate constant (3.75 × 10−4 cm s−1), and a low Tafel slope of 97 mV dec−1. To better measure intrinsic activity, we add a new descriptor, Jη = (Jₚ (peak current density)−Jₒₙₛₑₜ (onset current density)), which represents the net operating current above onset. Jη correlates strongly with traditional kinetic measurements, highlighting the conductivity-driven performance gain in HEO-10C (44.59 mA cm−2), which is about 1.6× greater than the uncoated HEO. These findings confirm graphite coating as a viable method for modifying multication HEO electrodynamics and introduce a new measure for assessing advanced oxide-based electrocatalysts.
Copyright (c) 2026 Shakeel Abbas, Akbar Hussain, Muhammad Asim, Tehmeena Maryum Butt, Banafsha Habib Ur Rehman, Javeria Arshad, Amina Hana, Sadia Kanwal, Muhammad Yasir, Naveed Kausar Janjua

This work is licensed under a Creative Commons Attribution 4.0 International License.
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