Anchoring the late first row transition metals with B12P12 nanocage to act as single atom catalysts toward oxygen evolution reaction (OER)

Allangawi, Abdulrahman; Mahmood, Tariq; Ayub, Khurshid; Gilani, Mazhar Amjad

doi:10.1016/j.mssp.2022.107164

Cited by 35 publications

(13 citation statements)

References 87 publications

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“…55 For the cases discussed here, the PDOS for these TMdoped graphene and the electric charge difference Dr TM indicate that the bonding is also formed from a hybridization scheme which involves involving the 3d, 4s, and 4p orbitals of the TM atom and the 2p orbitals from surrounding C atoms. However, in contrast to the previous studies, [51][52][53][54] electrons in these TM-doped graphene are much more delocalized, as implied by the local charge in each atom. Tables S1-S6 of ESI † indicates that the charges in each carbon atom and TM atom are smaller than their valence numbers, suggesting that a portion of electrons are largely delocalized around the TM dopant.…”

Section: Structure Optimization and Electronic Structurecontrasting

confidence: 92%

“…It is worthwhile to note that similar systems consisting of a single transition metal atom embedded in nano-molecules or two-dimensional architectures have been also reported, which are mainly intended for developing efficient catalytic materials. [51][52][53][54] In systems with low electron delocalization, the valence electrons from both TM and the ligand or surrounding atoms may form a bonding through several possible hybridization schemes leading to a typical trigonal bipyramidal or octahedral local coordination. In such cases, analysis of the ligand eld effect should be carefully undertaken, which may determine the orbital level splitting as well as the spin multiplicity.…”

Section: Structure Optimization and Electronic Structurementioning

confidence: 99%

“…The spin multiplicity may thus be neglected as a rst approximation, in contrast to the previous studies on the low electron delocalization systems. [51][52][53][54] For the TM-doped graphene considered in this work, it seems that spin multiplicity has a minor role in the electronic structure and the subsequence optical properties (see ESI Point no. 2 †).…”

Section: Structure Optimization and Electronic Structurementioning

confidence: 99%

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Modification of plasmonic properties in several transition metal-doped graphene studied by the first principles method

et al. 2023

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Section: Structure Optimization and Electronic Structurecontrasting

confidence: 92%

Section: Structure Optimization and Electronic Structurementioning

confidence: 99%

Section: Structure Optimization and Electronic Structurementioning

confidence: 99%

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Modification of plasmonic properties in several transition metal-doped graphene studied by the first principles method

et al. 2023

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“…In contrast, the 6-311G(d,p) basis set is chosen, which is a Pople-type basis set that contains the polarization function. The level of theory (ωB97XD/6-311G(d,p)) chosen here is well reported in literature, where it is used to investigate the potential of single-atom catalysis [ 68 ]. The frequency analysis is also performed to confirm the nature of the stationary points, such that the absence of the negative frequency validates the true minima nature of the reactants and products (stationary points) of all the studied TM@nanobelt analogues.…”

Section: Methodsmentioning

confidence: 99%

Hydrogen Dissociation Reaction on First-Row Transition Metal Doped Nanobelts

et al. 2023

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Zigzag molecular nanobelts have recently captured the interest of scientists because of their appealing aesthetic structures, intriguing chemical reactivities, and tantalizing features. In the current study, first-row transition metals supported on an H6-N3-belt[6]arene nanobelt are investigated for the electrocatalytic properties of these complexes for the hydrogen dissociation reaction (HDR). The interaction of the doped transition metal atom with the nanobelt is evaluated through interaction energy analysis, which reveals the significant thermodynamic stability of TM-doped nanobelt complexes. Electronic properties such as frontier molecular orbitals and natural bond orbitals analyses are also computed, to estimate the electronic perturbation upon doping. The highest reduction in the HOMO–LUMO energy gap compared to the bare nanobelt is seen in the case of the Zn@NB catalyst (4.76 eV). Furthermore, for the HDR reaction, the Sc@NB catalyst displays the best catalytic activity among the studied catalysts, with a hydrogen dissociation barrier of 0.13 eV, whereas the second-best catalytic activity is observed for the Zn@NB catalyst (0.36 eV). It is further found that multiple active sites, i.e., the presence of the metal atom and nitrogen atom moiety, help to facilitate the dissociation of the hydrogen molecule. These key findings of this study enhance the understanding of the relative stability, electronic features, and catalytic bindings of various TM@NB catalysts.

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“…The calculations are performed at the B3LYP/6-31G(d,p) level of theory. B3LYP is a well-documented DFT functional commonly employed for the computation of thermodynamic stabilities, electronic characteristics, and mechanistic studies of fullerenes. − Furthermore, a B3LYP functional is a proven accurate and a reliable functional in the field of SAC . Therefore, a B3LYP functional is chosen for geometry optimizations and energy profile analysis.…”

Section: Methodsmentioning

confidence: 99%

Metallofullerenes as Robust Single-Atom Catalysts for Adsorption and Dissociation of Hydrogen Molecules: A Density Functional Study

Sarfaraz,

Yar,

Hussain

et al. 2023

ACS Omega

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Hydrogen is currently considered as the best alternative for traditional fuels due to its sustainable and ecofriendly nature. Additionally, hydrogen dissociation is a critical step in almost all hydrogenation reactions, which is crucial in industrial chemical production. A cost-effective and efficient catalyst with favorable activity for this step is highly desirable. Herein, transition-metal-doped fullerene (TM@C60) complexes are designed and investigated as single-atom catalysts for the hydrogen splitting process. Interaction energy analysis (E int) is also carried out to demonstrate the stability of designed TM@C60 metallofullerenes, which reveals that all the designed complexes have higher thermodynamic stability. Furthermore, among all the studied metallofullerenes, the best catalytic efficiency for hydrogen dissociation is seen for the Sc@C60 catalyst E a = 0.13 eV followed by the V@C60 catalyst E a = 0.19 eV. The hydrogen activation and dissociation processes over TM@C60 metallofullerenes is further elaborated by analyzing charge transfer via the natural bond orbital and electron density difference analyses. Additionally, quantum theory of atoms in molecule analysis is carried out to investigate the nature of interatomic interactions between hydrogen molecules and TMs@C60 metallofullerenes. Overall, results of the current study declare that the Sc@C60 catalyst can act as a low cost, highly efficient, and noble metal-free single-atom catalyst to efficiently catalyze hydrogen dissociation reaction.

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Anchoring the late first row transition metals with B12P12 nanocage to act as single atom catalysts toward oxygen evolution reaction (OER)

Cited by 35 publications

References 87 publications

Modification of plasmonic properties in several transition metal-doped graphene studied by the first principles method

Modification of plasmonic properties in several transition metal-doped graphene studied by the first principles method

Hydrogen Dissociation Reaction on First-Row Transition Metal Doped Nanobelts

Metallofullerenes as Robust Single-Atom Catalysts for Adsorption and Dissociation of Hydrogen Molecules: A Density Functional Study

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