Optimising the platinum–carbon bond in nitrogen-doped single-walled carbon nanotubes

Improving Platinum Catalyst Durability with a Doped Graphene Support

“…These results are dependent on which dopant is employed as each element affects the local bonding in the surface in a unique way. The results given for the undoped and nitrogen-doped systems reported here are very different from those presented in our previous works; however, the trend remains unchanged. , Changing the basis set can have a profound effect on the magnitude of the result, as demonstrated in a work by Bühl et al The different functional and basis set combinations considered in this study on 25 third-row transition-metal complexes showed that the Lanl2DZ basis set was inferior to SDD based on the standard deviation of 41 metal–ligand distances. Lanl2DZ is a compact basis set, whereas SDD is more flexible, which decreases the variability in the metal–ligand distance.…”

“…Dunning 51 showed, while optimizing the structure of a single water molecule, that different basis set contractions can lead to a ground-state difference of as much as 0.99 eV. The binding energy between the Pt atom and the undoped graphene flake measured with Lanl2MB was −1.975 eV, 8 whereas using Lanl2DZ, it was −1.27 eV. 5 The differences between those two results and the undoped case here can be due to the change in basis set for the lighter elements (STO-3G for Lanl2MB, D95 V for Lanl2DZ, and 6-31G(d) in this work), as well as the difference in the effective core potential used.…”

“…One method is to modify the substrate by substituting carbon for other elements in the matrix, which will be referred to as doping. Using ab initio methods, it has been reported that various nitrogen- and boron-doping arrangements in graphene have a positive effect on the binding energy between platinum and the surface − and has also been extended to carbon nanotubes. − The link between binding energy and catalyst durability is substantiated by experimental evidence that nitrogen-doped fullerenes show an increase in dispersion of platinum, a resistance to agglomeration of nanoparticles, and a less significant deterioration of activity when compared with pure carbon cases. ,,− …”

One-dimensional nitrogen-containing carbon nanostructures

“…Hence, a good communication between theoreticians and experimentalists is absolutely necessary to resolve an important question of improved ORR activity of 1-D NCNSs.As the functionalization of NCNSs by metals is rather important for practical applications, there are a number of theoretical studies covering this area. Adsorption of Al[606], Pd[607], Pt[608,609] was investigated. Also, systematic studies of transition metals adsorption on SWNCNTs are available[610][611][612].…”