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Main Authors: Ipaves, Bruno, Justo, João F., de Almeida, James M., Assali, Lucy V. C., Autreto, Pedro Alves da Silva
Format: Preprint
Published: 2025
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Online Access:https://arxiv.org/abs/2502.10863
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author Ipaves, Bruno
Justo, João F.
de Almeida, James M.
Assali, Lucy V. C.
Autreto, Pedro Alves da Silva
author_facet Ipaves, Bruno
Justo, João F.
de Almeida, James M.
Assali, Lucy V. C.
Autreto, Pedro Alves da Silva
contents This study investigates the structural, electronic, and catalytic properties of pristine and doped C$_4$N$_2$ nanosheets as potential electrocatalysts for the hydrogen evolution reaction. The pristine C$_{36}$N$_{18}$ nanosheets exhibit limited HER activity, primarily due to high positive Gibbs free energies ($>$ 2.2 eV). To enhance catalytic performance, doping with B, Si, or P at the nitrogen site was explored. Among these systems, B-doped C$_{36}$N$_{17}$ nanosheets exhibit the most promising catalytic activity, with a Gibbs free energy close to zero ($\approx -0.2$ eV), indicating efficient hydrogen adsorption. Band structure, projected density of states, charge density, and Bader charge analyses reveal significant changes in the electronic environment due to doping. While stacking configurations (AA$'$A$''$ and ABC) have minimal effect on catalytic performance, doping -- particularly with B -- substantially alters the electronic structure, optimizing hydrogen adsorption and facilitating efficient HER. These findings suggest that B-doped C$_{36}$N$_{17}$ nanosheets could serve as efficient cocatalysts when combined with metallic materials, offering a promising approach to enhance catalytic efficiency in electrocatalytic and photocatalytic applications.
format Preprint
id arxiv_https___arxiv_org_abs_2502_10863
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Enhancing catalyst activity of two-dimensional C$_4$N$_2$ through doping for the hydrogen evolution reaction
Ipaves, Bruno
Justo, João F.
de Almeida, James M.
Assali, Lucy V. C.
Autreto, Pedro Alves da Silva
Materials Science
Computational Physics
This study investigates the structural, electronic, and catalytic properties of pristine and doped C$_4$N$_2$ nanosheets as potential electrocatalysts for the hydrogen evolution reaction. The pristine C$_{36}$N$_{18}$ nanosheets exhibit limited HER activity, primarily due to high positive Gibbs free energies ($>$ 2.2 eV). To enhance catalytic performance, doping with B, Si, or P at the nitrogen site was explored. Among these systems, B-doped C$_{36}$N$_{17}$ nanosheets exhibit the most promising catalytic activity, with a Gibbs free energy close to zero ($\approx -0.2$ eV), indicating efficient hydrogen adsorption. Band structure, projected density of states, charge density, and Bader charge analyses reveal significant changes in the electronic environment due to doping. While stacking configurations (AA$'$A$''$ and ABC) have minimal effect on catalytic performance, doping -- particularly with B -- substantially alters the electronic structure, optimizing hydrogen adsorption and facilitating efficient HER. These findings suggest that B-doped C$_{36}$N$_{17}$ nanosheets could serve as efficient cocatalysts when combined with metallic materials, offering a promising approach to enhance catalytic efficiency in electrocatalytic and photocatalytic applications.
title Enhancing catalyst activity of two-dimensional C$_4$N$_2$ through doping for the hydrogen evolution reaction
topic Materials Science
Computational Physics
url https://arxiv.org/abs/2502.10863