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

The geometries, electronic structures, and catalytic properties of BN-codoped fullerenes C59-nBNn (n = 1-3) are studied using first-principles computations. The results showed that BN-codoping can significantly modify the properties of C-60 fullerene by breaking local charge neutrality and creating active sites. The codoping of B and N enhances the formation energy of fullerenes, indicating that the synergistic effects of these atoms helps to stabilize the C59-nBNn structures. The stepwise addition of N atoms around the B atom improves catalytic activities of C59-nBNn in N2O reduction. The reduction of N2O over C58BN and C57BN2 begins with its chemisorption on the B-C bond of the fullerene, followed by the concerted interaction of CO with N2O and the release of N-2. The resulting OCO intermediate is subsequently transformed into a CO2 molecule, which is weakly adsorbed on the B atom of the fullerene. On the contrary, nitrogen-rich C56BN3 fullerene is found to decompose N2O into N-2 and O* species without the requirement for activation energy. The CO molecule then removes the O* species with a low activation barrier. The activation barrier of the N2O reduction on C56BN3 fullerene is just 0.28 eV, which is lower than that of noble metals.

Automated summary

The study on BN-codoped fullerenes C59-nBNn (n = 1-3) reveals that the synergistic effects of B and N atoms significantly modify the properties of the fullerenes, stabilize the structures, and enhance the catalytic activities. In N2O reduction, the addition of BN atoms in the fullerenes lowers the activation barrier, improving the reaction rate.