Ab initio insight into the electrolysis of water on basal and edge (fullerene C20) surfaces of 4 Å single-walled carbon nanotubes

Zhen Jiang; Nadia N. Intan; Qiong Yang

doi:10.1039/D2RA06123F

Ab initio insight into the electrolysis of water on basal and edge (fullerene C₂₀) surfaces of 4 Å single-walled carbon nanotubes†

Zhen Jiang,

*^a Nadia N. Intan

^b and Qiong Yang^c

Author affiliations

* Corresponding authors

^a Department of Chemistry, University of Pennsylvania, Philadelphia, PA 19104-6323, USA
E-mail: zjiang16@sas.upenn.edu

^b Department of Chemical and Biomolecular Engineering, University of Nebraska-Lincoln, Lincoln, NE 68588, USA

^c Hunan Provincial Key Laboratory of Thin Film Materials and Devices, School of Materials Science and Engineering, Xiangtan University, Xiangtan, Hunan 411105, China

Abstract

The extreme surface reactivity of 4 Å single-walled carbon nanotubes (SWCNTs) makes for a very promising catalytic material, however, controlling it experimentally has been found to be challenging. Here, we employ ab initio calculations to investigate the extent of surface reactivity and functionalization of 4 Å SWCNTs. We study the kinetics of water dissociation and adsorption on the surface of 4 Å SWCNTs with three different configurations: armchair (3,3), chiral (4,2) and zigzag (5,0). We reveal that out of three different configurations of 4 Å SWCNTs, the surface of tube (5,0) is the most reactive due to its small HOMO–LUMO gap. The dissociation of 1 H₂O molecule into an OH/H pair on the surface of tube (5,0) has an adsorption energy of −0.43 eV and an activation energy barrier of 0.66 eV at 298.15 K in pure aqueous solution, which is less than 10% of the activation energy barrier of the same reaction without the catalyst present. The four steps of H⁺/e⁻ transfer in the oxygen evolution reaction have also been studied on the surface of tube (5,0). The low overpotential of 0.38 V indicates that tube (5,0) has the highest potential efficiency among all studied carbon-based catalysts. We also reveal that the armchair edge of tube (5,0) is reconstructed into fullerene C₂₀. The dangling bonds on the surface of fullerene C₂₀ result in a more reactive surface than the basal surface of tube (5,0), however the catalytic ability was also inhibited in the later oxygen reduction processes.

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Article information

DOI: https://doi.org/10.1039/D2RA06123F
Article type: Paper
Submitted: 28 Sep 2022
Accepted: 10 Nov 2022
First published: 22 Nov 2022
This article is Open Access

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RSC Adv., 2022,12, 33552-33558

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Ab initio insight into the electrolysis of water on basal and edge (fullerene C₂₀) surfaces of 4 Å single-walled carbon nanotubes

Z. Jiang, N. N. Intan and Q. Yang, RSC Adv., 2022, 12, 33552 DOI: 10.1039/D2RA06123F

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