Potential of transition metal atoms embedded in buckled monolayer g-C₃N₄ as single-atom catalysts

Abstract

We use first-principles calculations to systematically explore the potential of transition metal atoms (Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Ru, Rh, Pd, Ag, Ir, Pt, and Au) embedded in buckled monolayer g-CN as single-atom catalysts. We show that clustering of Sc and Ti on g-CN is thermodynamically impeded and that V, Cr, Mn, and Cu are much less susceptible to clustering than the other TM atoms under investigation. Strong bonding of the transition metal atoms in the cavities of g-CN and high diffusion barriers together are responsible for single-atom fixation. Analysis of the CO oxidation process indicates that embedding of Cr and Mn in g-CN gives rise to promising single-atom catalysts at low temperature.

Single-Atom X/g-C3N4(X = Au1, Pd1, and Ru1) Catalysts for Acetylene Hydrochlorination: A Density Functional Theory Study

“…By placing the three investigated metals in all possible locations of the labeled atoms in g-C 3 N 4 Figure 1a, the three lowest energy structures of the catalysts were obtained. As shown in Figure 1b-d, Au, Pd, and Ru all tend to adsorb in a six-fold cavity of g-C 3 N 4 , which is consistent with a previous report [39]. The Au atom is located roughly in the middle of g-C 3 N 4 and is not connected to any other atom ( Figure 1b).…”

“…Their results showed that the resulting Cu-g-C 3 N 4 /AC catalyst displayed better catalytic performance than the aforementioned g-C 3 N 4 /AC catalyst. Moreover, the properties of the M/g-C 3 N 4 single-atom catalyst formed by embedding transition metal into monolayer g-C 3 N 4 were also examined [38,39]. All of the described studies encouraged us to embed the Au, Pd, and Ru metals in g-C 3 N 4 to form SACs for acetylene hydrochlorination reaction.…”

A Theory/Experience Description of Support Effects in Carbon-Supported Catalysts

“…In the context of CO oxidation, Cr and Mn can be considered as promising SAC since the metallic center adsorbs relatively weakly CO and O2 and the activation of the latter is reasonable energetically ~14-17 kcal.mol -1 . 312 Atomic cobalt incorporated in N-G has also been identified as active sites for the reduction of water to hydrogen, thanks to EXAFS. 313 Recently, Co1/N-G SAC has been also considered for dye-sensitized solar cells applications as counter electrode.…”

Recent Progress in Single‐Atom Catalysts for Photocatalytic Water Splitting

“…Graphitic carbon nitride (g-C 3 N 4 ) is currently regarded as a promising substrate material to anchor isolated metal atoms for photocatalysis, due to its high stability, abundant coordination sites, and visible-light response. [153][154][155][156][157][158][159][160][161][162][163] In the photocatalytic water-splitting system, the light absorption effect can be improved by single metal atoms supported on g-C 3 N 4 , which can be used as efficient active sites to boost reaction kinetics. Up to now, much research found that single-atom precious metals can be anchored onto g-C 3 N 4 for photocatalytic hydrogen evolution, which can effectively catalyze the photocatalytic water splitting into hydrogen.…”