Enhancing catalyst activity of two-dimensional C$_4$N$_2$ through doping for the hydrogen evolution reaction

Bruno Ipaves; João F. Justo; James M. de Almeida; Lucy V. C. Assali; Pedro Alves da Silva Autreto

doi:10.1021/acsomega.5c05773

paper

Enhancing catalyst activity of two-dimensional C $_{4}$ N $_{2}$ through doping for the hydrogen evolution reaction

arXiv:2502.10863 · doi:10.1021/acsomega.5c05773

Abstract

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.

Enhancing catalyst activity of two-dimensional C4​N2​ through doping for the hydrogen evolution reaction

Abstract

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Enhancing catalyst activity of two-dimensional C $_{4}$ N $_{2}$ through doping for the hydrogen evolution reaction