Al- or Si-decorated graphene oxide: A favorable metal-free catalyst for the N2O reduction

Esrafili, Mehdi D.; Sharifi, Fahimeh; Nematollahi, Parisa

doi:10.1016/j.apsusc.2016.06.127

Cited by 33 publications

(10 citation statements)

References 60 publications

(63 reference statements)

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“…Figure shows the most stable configuration of N 2 O molecule adsorbed over Si B and Si N . Our DFT calculations indicate N 2 O molecule prefers to be attached to the Si atom from its O‐site, an observation reported previously over other surfaces . Interestingly, N 2 O experiences a dissociative adsorption over both surfaces, in which it is spontaneously decomposed into N 2 molecule and an active oxygen atom (O ads ) adsorbed over the Si atom.…”

Section: Resultssupporting

confidence: 78%

“…Nitrous oxide (N 2 O) is a main greenhouse gas with important contribution to global warming, ozone depletion and acid rain formation . Hence, the development of efficient technology to control N 2 O emission has attracted much interest in recent years . The most commonly used approach to reduce N 2 O emission is its selective catalytic reduction with potential reducing agents.…”

Section: Introductionmentioning

confidence: 99%

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Single Si atom supported on defective boron nitride nanosheet as a promising metal‐free catalyst for N₂O reduction by CO or SO₂ molecule: A computational study

Esrafili

2018

Int J of Quantum Chemistry

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The low-temperature reduction of N 2 O plays a significant role for solving the growing environmental and health issues caused by emission of this greenhouse gas. The aim of this study is to investigate the possible reaction pathways for the reduction of N 2 O by CO or SO 2 molecule over Si-doped boron nitride nanosheet (Si-BNNS). According to our results, a B or N-vacancy defect in BN sheet could be able to greatly stabilize the single Si adatom. The relatively large diffusion barrier for the Si atom over the defective BN sheet also indicates Si-BNNS is stable enough to be utilized in catalytic reduction of N 2 O. The large charge-transfer from the surface to N 2 O leads to the spontaneous dissociation of this molecule into N 2 molecule and an activated oxygen atom (O ads ). The O ads moiety is then eliminated by CO or SO 2 molecule. The calculated activation energies and reaction energies reveal that the Si atom located on top of the B-vacancy site has a large catalytic activity toward the reduction of N 2 O by CO or SO 2 .adsorption, BN sheet, DFT, mechanism, N2O reduction 1 | I N TR ODU C TI ON Despite large efforts devoted to the development of renewable energy sources, fossil fuels now supply about 80% of the world's energy needs.However, these energy sources are closely linked with the emission of several hazardous gases, which contribute to undesirable health problems and climate changes. [1] Nitrous oxide (N 2 O) is a main greenhouse gas with important contribution to global warming, ozone depletion and acid rain formation. [2] Hence, the development of efficient technology to control N 2 O emission has attracted much interest in recent years. [3][4][5][6][7] The most commonly used approach to reduce N 2 O emission is its selective catalytic reduction with potential reducing agents. Among these, the catalytic reduction of N 2 O by CO molecule seems more effective, [8][9][10][11][12][13][14][15] since CO is cheap and readily available. Besides, this method is beneficial since toxic CO is removed from the atmosphere at the same time. However, sulfur dioxide (SO 2 ) is another important air pollutant, coming mainly from incomplete burning of fossil fuels in automobiles and industrial processes. [16] The most effective way to remove this hazardous gas has been proven to be its catalytic oxidation to SO 3 or other sulfur oxides before its emission. Accordingly, much attention has been recently paid to the low-temperature oxidation of SO 2 , due to its importance in solving the increasing environmental problems. [17][18][19][20][21][22][23] Though, considerable efforts have been devoted to oxidation of SO 2 by various noble metals. [24,25] However, these noble metal catalysts are scare, expensive and usually need high reaction temperature for efficient operation, which hinder their large-scale application. Therefore, the development of efficient metal-free catalysts for low-temperature oxidation of SO 2 remains a significant challenge.Recently, boron nitride (BN) nanomaterials have been widely studied as promi...

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Section: Resultssupporting

confidence: 78%

Section: Introductionmentioning

confidence: 99%

Single Si atom supported on defective boron nitride nanosheet as a promising metal‐free catalyst for N₂O reduction by CO or SO₂ molecule: A computational study

Esrafili

2018

Int J of Quantum Chemistry

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“…The decomposition barrier is also decreased monotonously with the increasing electric field, and there is no barrier while the intensity of the positive electric field is 0.5 V/Å. Using the DFT computational method, Mehdi et al [34] studied the reaction of reducing N 2 O by CO on the surfaces of the Al atom- or Si atom-decorated graphene oxide (Al–GO or Si–GO), where the results showed that the activation energy of the N 2 O decomposition process on Al–GO or Si–GO is almost negligible; the product N 2 can be easily desorbed from the surface, which indicates that both Al–GO and Si–GO can be served as promising alternatives to enhance the N 2 O adsorption and decomposition process.…”

Section: Introductionmentioning

confidence: 99%

DFT Study of N2O Adsorption onto the Surface of M-Decorated Graphene Oxide (M = Mg, Cu or Ag)

et al. 2019

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In order to reduce the harm of nitrous oxide (N2O) on the environment, it is very important to find an effective way to capture and decompose this nitrous oxide. Based on the density functional theory (DFT), the adsorption mechanism of N2O on the surfaces of M-decorated (M = Mg, Cu or Ag) graphene oxide (GO) was studied in this paper. The results show that the effects of N2O adsorbed onto the surfaces of Mg–GO by O-end and Cu–GO by N-end are favorable among all of the adsorption types studied, whose adsorption energies are −1.40 eV and −1.47 eV, respectively. Both adsorption manners belong to chemisorption. For Ag–GO, however, both the adsorption strength and electron transfer with the N2O molecule are relatively weak, indicating it may not be promising for N2O removal. Moreover, when Gibbs free energy analyses were applied for the two adsorption types on Mg–GO by O-end and Cu–GO by N-end, it was found that the lowest temperatures required to undergo a chemisorption process are 209 °C and 338 °C, respectively. After being adsorbed onto the surface of Mg–GO by O-end, the N2O molecule will decompose into an N2 molecule and an active oxygen atom. Because of containing active oxygen atom, the structure O–Mg–GO has strong oxidizability, and can be reduced to Mg–GO. Therefore, Mg–GO can be used as a catalyst for N2O adsorption and decomposition. Cu–GO can be used as a candidate material for its strong adsorption to N2O.

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“…[7][8][9][10][11][12] The pristine graphene (p-GN) in the ground state was firstly tested finding no catalytic effects. As reported, the adsorption and catalytic performances of graphene are regulated effectively by doping [28][29][30] or excitation, [31][32][33][34] while neither of these strategies seems valid for the present catalytic processes. Doping and photocatalysis through excitations were then combined for catalyst designs, which demonstrate the gratifying results: All the elementary steps for N 2 O decomposition and benzene hydroxylation proceed with moderate energy barriers, indicating the facile manufacturing of phenol under mild conditions.…”

Section: Introductionmentioning

confidence: 99%

Facile and Direct Hydroxylation of Benzene to Phenol over Graphene‐Based Catalysts: Integrated Utilization of Greenhouse Nitrous Oxide

Zhu

Yun

Wang

et al. 2018

Advcd Theory and Sims

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Graphene catalysis has recently emerged as a focus and herein a novel and highly efficient process is computationally designed using graphene-based catalysts that integrates the utilization of greenhouse nitrous oxide (N 2 O) as oxidant. The ground-state pristine graphene is not catalytically active for benzene hydroxylation, and doping and photocatalysis through excitations are employed to improve the catalyst systems, while both strategies exhibit limited effects. A combination of Be-doping and photocatalysis through excitations results in encouraging changes, where all energy barriers are moderate, so that the whole catalytic processes proceed facilely at mild conditions. Graphene materials, especially Be-and O-doped ones, are good photocatalysts due to the low excitation energies. Mechanistic studies indicate that the active sites of the excited-state graphene, whether pristine or doped, are oxygen anion radical (O −• ) and distinct from the epoxide species for the ground state; in addition, Be-doping pronouncedly reduces the excitation energies and enhances the interactions with the active-site O species, which further show strong stabilization effects to transition states and reduce substantially the energy barriers.

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Al- or Si-decorated graphene oxide: A favorable metal-free catalyst for the N2O reduction

Cited by 33 publications

References 60 publications

Single Si atom supported on defective boron nitride nanosheet as a promising metal‐free catalyst for N₂O reduction by CO or SO₂ molecule: A computational study

Single Si atom supported on defective boron nitride nanosheet as a promising metal‐free catalyst for N₂O reduction by CO or SO₂ molecule: A computational study

DFT Study of N2O Adsorption onto the Surface of M-Decorated Graphene Oxide (M = Mg, Cu or Ag)

Facile and Direct Hydroxylation of Benzene to Phenol over Graphene‐Based Catalysts: Integrated Utilization of Greenhouse Nitrous Oxide

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Al- or Si-decorated graphene oxide: A favorable metal-free catalyst for the N2O reduction

Cited by 33 publications

References 60 publications

Single Si atom supported on defective boron nitride nanosheet as a promising metal‐free catalyst for N2O reduction by CO or SO2 molecule: A computational study

Single Si atom supported on defective boron nitride nanosheet as a promising metal‐free catalyst for N2O reduction by CO or SO2 molecule: A computational study

DFT Study of N2O Adsorption onto the Surface of M-Decorated Graphene Oxide (M = Mg, Cu or Ag)

Facile and Direct Hydroxylation of Benzene to Phenol over Graphene‐Based Catalysts: Integrated Utilization of Greenhouse Nitrous Oxide

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Single Si atom supported on defective boron nitride nanosheet as a promising metal‐free catalyst for N₂O reduction by CO or SO₂ molecule: A computational study

Single Si atom supported on defective boron nitride nanosheet as a promising metal‐free catalyst for N₂O reduction by CO or SO₂ molecule: A computational study