Nitrogen‐doped C₆₀ as a robust catalyst for CO oxidation

Abstract

The O activation and CO oxidation on nitrogen-doped C N fullerene are investigated using first-principles calculations. The calculations indicate that the C N fullerene is able to activate O molecules resulting in the formation of superoxide species ( O2-) both kinetically and thermodynamically. The active superoxide can further react with CO to form CO via the Eley-Rideal mechanism by passing a stepwise reaction barrier of only 0.20 eV. Ab initio molecular dynamics (AIMD) simulation is carried out to evidence the feasibility of the Eley-Rideal mechanism. In addition, the second CO oxidation takes place with the remaining atomic O without any activation energy barrier. The full catalytic reaction cycles can occur energetically favorable and suggest a two-step Eley-Rideal mechanism for CO oxidation with O catalyzed by the C N fullerene. The catalytic properties of high percentage nitrogen-doped fullerene (C N ) is also examined. This work contributes to designing higher effective carbon-based materials catalysts by a dependable theoretical insight into the catalytic properties of the nitrogen-doped fullerene. © 2017 Wiley Periodicals, Inc.

C59N Heterofullerene: A Promising Catalyst for NO Conversion into N2O

“…Besides, due to their curvature and pentagon defect compared with graphene, small porous nitrogen‐doped fullerenes have proven to exhibit rather high catalytic activity towards these reactions . A recent density functional theory (DFT) study by Lin and coworkers has shown that the incorporation of a nitrogen atom in C 60 , could greatly enhance the catalytic performance of this material towards the CO oxidation reaction. Chen and coworkers have also found that small N‐doped fullerenes C 59 N and C 39 N exhibit superior catalytic activity in the reduction of O 2 with energy barriers close to those on Pt (111).…”

“…As evident, the spin density mostly accumulates over the carbon atom (C1) nearest to the nitrogen. According to the previous studies, such a large spin density over the mentioned site can considerably facilitate the adsorption of O 2 molecule and lower the reaction barriers for its catalytic reduction. Likewise, this atomic site is expected as the most active site to interact with the NO molecule, which will be discussed below.…”

CO oxidization catalyzed by B, N, and their co-doped fullerenes: a first-principles investigation

“…The bonding between O and C 59 B results in a charge transfer of approximately 0.86e (calculated using the Bader analysis technique 46 ) from C 59 B to O 2 to elongate the O-O bond by 0.19Å to activate the O 2 , which is close to previously reported results. 33,[47][48][49] In our calculation, the O 2 is found in the 3 S g À triplet ground state before adsorption onto C 59 B. When it gets close enough to C 59 B to adsorb onto it, a charge transfer would occur.…”

“…Chen and his co-workers reported DFT studies on CO oxidizations catalyzed by N doped C 60 (ref. 33) and penta-graphene. 34 In addition, B, N, P, and Si-doped graphene also shows superior reactivities for catalyzing CO oxidizations.…”

Reversible CO2storage and efficient separation using Ca decorated porphyrin-like porous C24N24fullerene: a DFT study

“…11,12 These structures are also well suited for use as a support in heterogeneous catalysis due to their huge specic area. [13][14][15] The ability to tune the electronic and surface properties of carbon-based nanomaterials by introducing defects or heteroatoms has shed light on their potential use in sensors and energy technologies. [16][17][18][19] Theoretical calculations [20][21][22] and experimental investigations, 23,24 for example, have demonstrated that N atoms may be effectively incorporated in different carbon materials, tailoring their chemical and electronic characteristics.…”