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Context <p>To improve the efficiency of CO<sub>2</sub> adsorption in buckminsterfullerene (C<sub>60</sub>) is necessary to better understand and tune its properties. Replacing a carbon atom by a heteroatom with a strong Lewis acidity inside the pristine C<sub>60</sub> fullerene or applying an electric field can cause the nanostructure to become a high-performance CO<sub>2</sub> sorbent. In this theoretical study C<sub>60</sub> was doped by single boron atom to generate a fullerene (referred to as C<sub>59</sub>B). Minimum energies (the most stable 3D arrangement of the molecules) of C<sub>60</sub>-CO<sub>2</sub> and C<sub>59</sub>B-CO<sub>2</sub> systems were optimized using density functional theory (DFT) calculations to determine the adsorption energy and evaluate its stability. The influence of an external electric field (imposed in the direction of the axis passing through fullerene C<sub>60</sub> or C<sub>59</sub>B and CO<sub>2</sub> in the range of 0.001 and 0.020 au) in the CO<sub>2</sub> adsorption on C<sub>60</sub> and C<sub>59</sub>B was also studied. The adsorption energies of CO<sub>2</sub> on C<sub>60</sub> and C<sub>59</sub>B fullerenes were -0.14 and -0.21&#xa0;eV respectively, revealing the effect of the heteroatom dopant on the C<sub>59</sub>B with increasing adsorption energy. When applying an electric field of 0.011 au in C<sub>60</sub>-CO<sub>2</sub> and in C<sub>59</sub>B-CO<sub>2</sub>, the result was an adsorption energy of -0.3 and -1.2&#xa0;eV, respectively: providing higher performance for the C<sub>59</sub>B-CO<sub>2</sub> by increasing further the adsorption energy in this doped fullerene. Also, according to these results, the C–C bond formed between the CO<sub>2</sub> and the C<sub>59</sub>B fullerene applying electric field is covalent (1.7&#xa0;Å), which results in chemisorption. Additionally, the structural and electronic properties were studied, such as the dipole moment, electrostatic potential surfaces, the HOMO–LUMO gaps, the infrared (IR) spectrums were calculated to validate the stability of the molecular structures, and density of states (DOS) analysis to confirm the CO<sub>2</sub> adsorption on C<sub>60</sub> and on C<sub>59</sub>B and understand their interaction mechanism for possible applications such as CO<sub>2</sub> gas sensing or environmental remediation.</p> Methods <p>The geometry optimization and electronic properties calculations based on DFT were performed using ORCA software package. The computational parameters included the general gradient approximation functional PBE with 6—31G(<i>d</i>,<i>p</i>) basis set, combined with dispersion correction developed by Grimme DFT-D3 approach dispersion correction D3BJ and basis set superposition error (BSSE).</p> Graphical Abstract <p></p>

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Effect of boron-doping and electric field on CO2 adsorption on C60 fullerene. A DFT study

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年5月19日

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  • Miguel del Carmen Domínguez-Trujillo,
  • Alejandro Dorazco-González,
  • Humberto Julián Mandujano-Ramírez,
  • José Enrique Flores-Chan,
  • Juan Manuel Tadeo Sierra-Grajeda,
  • Sergio Martinez-Vargas

摘要

Context

To improve the efficiency of CO2 adsorption in buckminsterfullerene (C60) is necessary to better understand and tune its properties. Replacing a carbon atom by a heteroatom with a strong Lewis acidity inside the pristine C60 fullerene or applying an electric field can cause the nanostructure to become a high-performance CO2 sorbent. In this theoretical study C60 was doped by single boron atom to generate a fullerene (referred to as C59B). Minimum energies (the most stable 3D arrangement of the molecules) of C60-CO2 and C59B-CO2 systems were optimized using density functional theory (DFT) calculations to determine the adsorption energy and evaluate its stability. The influence of an external electric field (imposed in the direction of the axis passing through fullerene C60 or C59B and CO2 in the range of 0.001 and 0.020 au) in the CO2 adsorption on C60 and C59B was also studied. The adsorption energies of CO2 on C60 and C59B fullerenes were -0.14 and -0.21 eV respectively, revealing the effect of the heteroatom dopant on the C59B with increasing adsorption energy. When applying an electric field of 0.011 au in C60-CO2 and in C59B-CO2, the result was an adsorption energy of -0.3 and -1.2 eV, respectively: providing higher performance for the C59B-CO2 by increasing further the adsorption energy in this doped fullerene. Also, according to these results, the C–C bond formed between the CO2 and the C59B fullerene applying electric field is covalent (1.7 Å), which results in chemisorption. Additionally, the structural and electronic properties were studied, such as the dipole moment, electrostatic potential surfaces, the HOMO–LUMO gaps, the infrared (IR) spectrums were calculated to validate the stability of the molecular structures, and density of states (DOS) analysis to confirm the CO2 adsorption on C60 and on C59B and understand their interaction mechanism for possible applications such as CO2 gas sensing or environmental remediation.

Methods

The geometry optimization and electronic properties calculations based on DFT were performed using ORCA software package. The computational parameters included the general gradient approximation functional PBE with 6—31G(d,p) basis set, combined with dispersion correction developed by Grimme DFT-D3 approach dispersion correction D3BJ and basis set superposition error (BSSE).

Graphical Abstract