Abstract
Immobilization of two single transition metal (TM) atoms on a substrate host opens numerous possibilities for catalyst design. If the substrate contains more than one vacancy site, the combination of TMs along with their distribution patterns becomes a design parameter potentially complementary to the substrate itself and the bi-metal composition. By means of DFT calculations, we modeled three dissimilar bi-metal atoms (Ti, Mn, and Cu) doped into the six porphyrin-like cavities of porous C24N24 fullerene, considering different bi-metal distribution patterns for each binary complex, viz. TixCuz@C24N24, TixMny@C24N24, and MnyCuz@C24N24 (with x, y, z = 0–6). We elucidate whether controlling the distribution of bi-metal atoms into the C24N24 cavities can alter their catalytic activity toward CO2, NO2, H2, and N2 gas capture. Interestingly, Ti2Mn4@C24N24 and Ti2Cu4@C24N24 complexes showed the highest activity and selectively toward gas capture. Our findings provide useful information for further design of novel few-atom carbon-nitride-based catalysts.
Highlights
Porous carbon-based catalysts are widely used as sorbents and support materials in heterogeneous catalysis [1,2,3]
We investigate the catalytic activity of bi-metal atom doping in C24 N24, using Ti, Mn, and Cu as metals
We considered a combination of two metal atoms for the selected Ti, Mn, and Cu transition metal (TM) with 3d2 4s2, 3d5 4s2, and 3d10 4s1 valence electrons, respectively, i.e., TiCu, TiMn, and MnCu
Summary
Porous carbon-based catalysts are widely used as sorbents and support materials in heterogeneous catalysis [1,2,3]. The archetypical example is C60 fullerene, which has a closed-cage structure and can be synthesized with a highly defective surface and abundant holes [4,5] It has high thermal stability, unique mechanical properties, high electronegativity, and high electron affinity [6]. Chen et al [14] theoretically investigated the oxygen reduction reaction (ORR) mechanisms and catalytic abilities of pure and N-doped fullerenes of various sizes (C20 , C40 , C60 , and C180 ). Zhai et al [18] for the first time synthesized metal-free N-doped graphene films on glass through plasma-assisted hot filament CVD using N2 gas as dopant They found that both the hot filament and plasma. Our calculations can provide the fundamental adsorption mechanism of such a novel material, supporting its possible exploitation to be applied as a green catalyst for gas detection
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