Doped h-BN monolayer as efficient noble metal-free catalysts for CO oxidation: the role of dopant and water in activity and catalytic de-poisoning

Sinthika, S.; Kumar, E. Mathan; Thapa, Ranjit

doi:10.1039/c4ta02434f

Cited by 75 publications

(51 citation statements)

References 46 publications

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“…active sites. 13 29,53 In order to give a good measure of the intrinsic ability of h-BNNS/Cu(111) to catalyze CO oxidation, the Sabatier activity was also deduced following the previous theoretical studies. 6, the CO molecule is initially adsorbed near O* (IS2) with C-O* distance of 2.63 Å and the distance between h-BNNS and the first metal layer is about 2.51 Å.…”

Section: Activity Of Co Oxidation On H-bnns/cu(111)mentioning

confidence: 99%

A Cu(111) supported h-BN nanosheet: a potential low-cost and high-performance catalyst for CO oxidation

Lin

Huang

Gao

2015

Phys. Chem. Chem. Phys.

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A Cu(111) supported h-BN nanosheet (h-BNNS) has been systematically investigated by first-principles DFT using dispersion corrections. During the interaction between Cu and h-BNNS, the electrons migrate from the metal to the h-BNNS, leading to the formation of gap states above and under the Fermi level. Significant electrons are observed to migrate from the supported h-BNNS to the O2 molecule, resulting in the activation of the adsorbed O2. While for the unsupported h-BNNS, the absorbed O2 is almost intact with a very weak binding energy. CO oxidation is chosen as a benchmark probe reaction to better understand the enhanced catalytic activity induced by the Cu(111) metal substrate. The calculated energy barrier of the reaction CO + O2* → CO2* + O* is found to be only 0.51 eV with a large exothermicity of -2.93 eV. Even for the process of CO reacting with the residual atomic O* to generate CO2*, the barrier is found to be nearly null, helping the catalyst to facilely recover itself. Our calculation results suggest that the Cu(111) supported h-BNNS is a potential low cost and high activity catalyst for CO oxidation.

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Section: Activity Of Co Oxidation On H-bnns/cu(111)mentioning

confidence: 99%

A Cu(111) supported h-BN nanosheet: a potential low-cost and high-performance catalyst for CO oxidation

Lin

Huang

Gao

2015

Phys. Chem. Chem. Phys.

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“…On pure h-BN surface the energy required to dissociate the H 2 molecule into two H atoms is more than 2.29 eV, suggesting that dissociation at ordinary temperatures is quite unlikely. 41 In order to calculate the dissociation barrier, we performed Black dotted line is for guide to the eye to show nearest active sites. 57 However, in our case the doped COBN system is itself acting as a catalyst.…”

Section: Bond Exchange Mechanismmentioning

confidence: 99%

First principles guide to tune h-BN nanostructures as superior light-element-based hydrogen storage materials: role of the bond exchange spillover mechanism

2015

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We investigate the interaction of molecular hydrogen with light element based ndoped hexagonal boron nitride (h-BN) nanostructures and moreover explore the bond exchange mechanism for spillover of atomic hydrogen using dispersion-corrected density functional theory (DFT-D) calculations. A number of doped configurations were tested and it has been found that co-doping of C and O on h-BN sheet significantly increases the adsorption energy of molecular H 2 . The charge transfer from the n-doped h-BN surface to H 2 is found to be the reason for the higher interactions that boosted the binding energy. In addition, the doped h-BN surfaces act as catalysts and dissociate the H 2 molecule with very low activation barrier, but the migration of the resulting H atoms on the surface requires high energy. In order to facilitate easy and fast migration of H atoms, we introduce the bond exchange mechanism using external mediators i.e. borane (BH 3 ) and gallane (GaH 3 ) molecules which serve as a secondary catalysts and help in lowering the migration barrier, leading to the formation of hydrogenated surface. The partially hydrogenated surface in turn can also act as a hydrogen storage material, with a higher propensity to adsorb hydrogen molecules when compared to the unhydrogenated surface. Hence the surface proposed in this work can be used to store substantial quantity of hydrogen as energy source with easy adsorption and desorption kinetics.

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“…77 It is noticeable that the higher the Sabatier activity, the more favorable the mechanism. It is found that the Sabatier activity for the TER mechanism is 1.16 eV at room temperature, which is higher than those for the LH (1.00 eV) and ER (À0.39 eV) mechanisms.…”

Section: Co Oxidation Over Ag 1 -V B /Bnmentioning

confidence: 99%

A promising single atom catalyst for CO oxidation: Ag on boron vacancies of h-BN sheets

Yang

et al. 2017

Phys. Chem. Chem. Phys.

103

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Single atom catalysts (SACs) have attracted broad research interest in recent years due to their importance in various fields, such as environmental protection and energy conversion. Here, we discuss the mechanisms of CO oxidation to CO 2 over single Ag atoms supported on hexagonal boron-nitride sheets (Ag 1 /BN) through systematic van der Waals inclusive density functional theory (DFT-D)calculations. The Ag adatom can be anchored onto a boron defect (V B ), as suggested by the large energy barrier of 3.12 eV for Ag diffusion away from the V B site. Three possible mechanisms (i.e., Eley-Rideal, Langmuir-Hinshelwood, and termolecular Eley-Rideal) of CO oxidation over Ag 1 /BN are investigated. Due to ''CO-Promoted O 2 Activation'', the termolecular Eley-Rideal (TER) mechanism is the most relevant one for CO oxidation over Ag 1 /BN and the rate-limiting reaction barrier is only 0.33 eV. More importantly, the first principles molecular dynamics simulations confirm that CO oxidation via the TER mechanism may easily occur at room temperature. Analyses with the inclusion of temperature and entropy effects further indicate that the CO oxidation via the TER mechanism over Ag 1 /BN is thermodynamically favorable in a broad range of temperatures.

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Doped h-BN monolayer as efficient noble metal-free catalysts for CO oxidation: the role of dopant and water in activity and catalytic de-poisoning

Cited by 75 publications

References 46 publications

A Cu(111) supported h-BN nanosheet: a potential low-cost and high-performance catalyst for CO oxidation

A Cu(111) supported h-BN nanosheet: a potential low-cost and high-performance catalyst for CO oxidation

First principles guide to tune h-BN nanostructures as superior light-element-based hydrogen storage materials: role of the bond exchange spillover mechanism

A promising single atom catalyst for CO oxidation: Ag on boron vacancies of h-BN sheets

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