C₅₉X Heterofullerenes (X=N, B, Si, P and S) as Catalysts for Reduction of N₂O: A Comparative DFT Study

Abstract

Using DFT calculations, the adsorption behavior of N 2 O and CO molecules is studied over some C 59 X heterofullerenes (X = N, B, P, Si and S). The adsorption energies of N 2 O over C 59 X fullerenes are in the range of À 0.08 to À 1.73 eV (at the PBE/DNP level), while those of CO molecule range from À 0.06 to À 0.91 eV. Our results indicate that the tendency of C 59 B and C 59 Si to adsorb N 2 O and CO molecules is much larger than that of other heterofullerenes. The activation energy for the reduction of N 2 O by CO over C 59 Si is calculated to be only 0.15 eV. According to these results, C 59 Si can be regarded as a promising metalfree catalyst for low-temperature reduction of N 2 O.[a] Prof.

Electrochemical reduction of NO catalyzed by boron-doped C60 fullerene: a first-principles study

“…Doping of the B atom resulted in a small distortion around the dopant atom, which is consistent with the prior studies. 55,65,66 As seen in Fig. 1 , the C–C bond lengths surrounding the dopant atom are nearly equal to those of pure C 60 .…”

“…52,53 Consequently, C 59 B may adsorb small gas molecules such as O 2 , CO, and N 2 O due to the buildup of high spin density and relatively large positive charges over the B atom. [53][54][55] Likewise, the metal-free C 59 B is expected to be a very active catalyst for NO adsorption and electrochemical reduction. However, no theoretical or experimental studies on the catalytic reactivity of C 59 B for the NOER process have been conducted.…”

Synergic effects between boron and nitrogen atoms in BN-codoped C59−nBNnfullerenes (n= 1–3) for metal-free reduction of greenhouse N2O gas

“…Due to large activation of N 2 O on the C 57 BN 2 , a relatively smaller E bar is obtained (0.36 eV), which is comparable to the mentioned value for the Fe-doped graphene (0.83 eV). 86 Also, these E bar values are lower than that of over C 59 B (1.95 eV), 88 suggesting that the BN codoping is able to substantially improve the catalytic properties of the C 60 fullerene. In the next step, the OCO is converted to CO 2 molecule as shown in Fig.…”

Local Aromaticity: An Important Indicator of the Surface Active Sites of Heterocyclic Nanostructures

“…The reported adsorption sites of different species on their surfaces are summarized in Table S1. For B C –C 60 , the doped B site is the best choice for adsorbing molecules such as NO 2 , O 2 , NO, N 2 O, CO, OH, and OOH. − Similarly, P C –C 60 ,, and Si C –C 60 ,, are both reported to favor the adsorption of O 2 , CO, OH, and OOH at the site of doped atom. In contrast, the carbon site adjacent to the doped N atom is well recognized as the optimal site for NO 2 , O 2 , NO, N 2 O, CO, H, OH, COOH, and OOH in N C –C 60 . ,− Figure clearly shows that all the surface sites with the strongest antiaromaticity on the doped C 60 are exactly the ones reported in the literature.…”