DFT study on CO2 capture using boron, nitrogen, and phosphorus-doped C20 in the presence of an electric field
Parham Rezaee, Shervin Alikhah Asl, Mohammad Hasan Javadi, Shahab Rezaee, Razieh Morad, Mahmood Akbari, Seyed Shahriar Arab, Malik Maaza
Abstract
Abstract Burning fossil fuels emits a significant amount of $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> , causing climate change concerns. $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> Capture and Storage (CCS) aims to reduce emissions, with fullerenes showing promise as $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> adsorbents. Recent research focuses on modifying fullerenes using an electric field. In light of this, we carried out DFT studies on some B, N, and P doped $$\hbox {C}_{20}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>C</mml:mtext> <mml:mn>20</mml:mn> </mml:msub> </mml:math> ( $$C_{20-n}X_n$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mmultiscripts> <mml:mi>C</mml:mi> <mml:mrow> <mml:mn>20</mml:mn> <mml:mo>-</mml:mo> <mml:mi>n</mml:mi> </mml:mrow> <mml:mrow/> </mml:mmultiscripts> <mml:msub> <mml:mi>X</mml:mi> <mml:mi>n</mml:mi> </mml:msub> </mml:mrow> </mml:math> , n = 0, 1, 2, and 3; X = B, N, and P) in the absence and presence of an electric field in the range of 0-0.02 a . u .. The cohesive energy was calculated to ensure their thermodynamic stability showing, that despite having lesser cohesive energies than $$\hbox {C}_{20}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>C</mml:mtext> <mml:mn>20</mml:mn> </mml:msub> </mml:math> , they appear in a favorable range. Moreover, the charge distribution for all structures was depicted using the ESP map. Most importantly, we evaluated the adsorption energy, height, and $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> angle, demonstrating the B and N-doped fullerenes had the stronger interaction with $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> , which by far exceeded $$\hbox {C}_{20}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>C</mml:mtext> <mml:mn>20</mml:mn> </mml:msub> </mml:math> ’s, improving its physisorption to physicochemical adsorption. Although the adsorption energy of P-doped fullerenes was not as satisfactory, in most cases, increasing the electric field led to enhancing $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> adsorption and incorporating chemical attributes to $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> -fullerene interaction. The HOMO–LUMO plots were obtained by which we discovered that unlike the P-doped $$\hbox {C}_{20}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>C</mml:mtext> <mml:mn>20</mml:mn> </mml:msub> </mml:math> , the surprising activity of B and N-doped $$\hbox {C}_{20}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>C</mml:mtext> <mml:mn>20</mml:mn> </mml:msub> </mml:math> s against $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> originates from a high concentration of the HOMO-LUMO orbitals on B, N and neighboring atoms. In the present article, we attempt to introduce more effective fullerene-based materials for $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> adsorption as well as strategies to enhance their efficiency and revealing adsorption nature over B, N, and P-doped fullerenes and in the end, hope to encourage more experimental research on these materials within growing electric field for $$\hbox {CO}_{2}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:msub> <mml:mtext>CO</mml:mtext> <mml:mn>2</mml:mn> </mml:msub> </mml:math> capture in the future.