Perspectives on Electron Transfer Kinetics Across Graphene-Family Nanomaterials and the Interplay of Electronic Structure with Defects and Quantum Capacitance - Publication - Bridge of Knowledge

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Perspectives on Electron Transfer Kinetics Across Graphene-Family Nanomaterials and the Interplay of Electronic Structure with Defects and Quantum Capacitance

Abstract

This perspective presents a combined experimental-theory investigation of the mechanistic outer-sphere electron transfer (OS-ET) kinetics in an adiabatic regime for a cornerstone electrochemical reaction, fundamental to efficient energy interconversion as in electrochemical double layer supercapacitors, across graphene-family nanomaterials (GFNs) ranged from pristine graphene to nitrogen-doped graphene aerogel and the novel laser-induced graphene. Using scanning electrochemical microscopy (SECM) operating in feedback mode and co-located spectroscopy, the ET rate constant, k0 (or kET, cm/s) was quantified while imaging electroactivity of OS potassium hexacyanoferrate (III/IV) [Fe (CN)64-/3-] or ferrocene methanol [Fc0/Fc+] redox probe yielding unexpected trends. We examined factors affecting the kinetic rate constant rationalized through physical model and parameterized using density functional theory with incorporation of defects and dopant. We attributed the improved kinetic rates (0.010.1 via SECM) compared with ensemble-averaged method (0.0010.01 cm/s) to pointlike topological defects in basal plane (number density ~1012/cm2), oxygen functional groups (C/O ratio: 4:112:1) and nitrogen doping, edge plane hydrogen-bonding sites (density: 0.11.0 μm-1), altered electronic structure factored into available density of states near Fermi level (-0.2+0.2 eV), and quantum capacitance. We elucidated the ET kinetics tunability by engineering the electronic band structure, varying electrode potential, and morphological diversity.

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DOI:
Digital Object Identifier (open in new tab) 10.1038/s41598-025-04357-x
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Category:
Articles
Type:
artykuły w czasopismach
Published in:
Scientific Reports no. 15, pages 1 - 15,
ISSN: 2045-2322
Language:
English
Publication year:
2025
Bibliographic description:
Gupta S., Narajczyk M., Sawczak M., Bogdanowicz R.: Perspectives on Electron Transfer Kinetics Across Graphene-Family Nanomaterials and the Interplay of Electronic Structure with Defects and Quantum Capacitance// Scientific Reports -, (2025), s.1-15
DOI:
Digital Object Identifier (open in new tab) 10.1038/s41598-025-04357-x
Sources of funding:
  • IDUB
Verified by:
Gdańsk University of Technology

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