Effect of sulfation on the surface activity of CaO for N2O decomposition

Wu, Lingnan; Hu, Xiaoying; Wu, Qin; Chen, Dong; Yang, Yongping

doi:10.1016/j.apsusc.2015.09.006

Cited by 7 publications

(7 citation statements)

References 39 publications

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“…To select a proper model for the Cu 2 O surface, the surface energies (σ sur ) of Cu 2 O low‐index facets were studied first according to Eq. :

\begin{matrix} true \\ right σ_{sur} = \frac{E_{slab} - N E_{bulk}}{2 A_{sur}} \end{matrix}

…”

Section: Methodsmentioning

confidence: 99%

Mechanism of CO Oxidation on Cu₂O (111) Surface: A DFT and Microkinetic Study

Tian

2018

Int J of Chemical Kinetics

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Catalytic oxidation has been recognized as one of the most efficient and promising techniques for the abatement of CO and volatile organic compounds. In the present work, the CO oxidation mechanism on perfect Cu2O (111) surface was investigated by using density functional theory (DFT) calculations with the periodic surface model. The unsaturated singly coordinated Cu+ site of Cu2O (111) surface could effectively adsorb gaseous CO molecule with a strong adsorption energy of −1.558 eV. The adsorbed O on Cu2O (111) surface is very active toward CO oxidation with only 0.269 eV energy barrier. The reaction between CO and lattice O is the rate‐determining step of Mars‐van‐Krevelen (MvK) type CO oxidation with the energy barrier of 1.629 eV. The CO oxidation cycle initiated by the reaction between coadsorbed CO and O2 at the CuI site has a relatively lower energy barrier of 1.082 eV and is, therefore, more likely to proceed compared with the MvK cycle. Microkinetic rate constants of elementary reaction steps based on the transition state theory were deduced, which could be helpful in the kinetic modeling of CO oxidation on Cu2O surface.

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“…To select a proper model for the Cu 2 O surface, the surface energies (σ sur ) of Cu 2 O low‐index facets were studied first according to Eq. :

\begin{matrix} true \\ right σ_{sur} = \frac{E_{slab} - N E_{bulk}}{2 A_{sur}} \end{matrix}

…”

Section: Methodsmentioning

confidence: 99%

Mechanism of CO Oxidation on Cu₂O (111) Surface: A DFT and Microkinetic Study

Tian

2018

Int J of Chemical Kinetics

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“…The limestone is converted into CaSO 4 by the reaction of calcium oxide (CaO) with sulfur oxides (SO x ) and oxygen (O 2 ), removing sulfur oxides from the system. According to a previous study, some free CaO surfaces cause the decomposition of N 2 O, through the catalytic reaction with the N 2 O . Influence of limestone and calcium carbonate on the N 2 O and NO concentrations have been actively studied for power plants with high N 2 O concentrations. − Through laboratory-scale reactor experiments, calcium carbonate was found to act as a strong catalyst in the decomposition of N 2 O. − As the CaO content of ash among the filler inside the furnace of CFBC increases, the catalytic decomposition of N 2 O increases. , The reaction catalyzed on the CaO surface is shown in the following equation …”

Section: Research Resultsmentioning

confidence: 99%

“…According to a previous study, some free CaO surfaces cause the decomposition of N 2 O, through the catalytic reaction with the N 2 O. 12 Influence of limestone and calcium carbonate on the N 2 O and NO concentrations have been actively studied for power plants with high N 2 O concentrations. 13−19 Through laboratory-scale reactor experiments, calcium carbonate was found to act as a strong catalyst in the decomposition of N 2 O.…”

Section: Methodsmentioning

confidence: 99%

Study on the Variance of N₂O Concentration after Air Pollution Prevention Facility in Bituminous Coal-Firing Power Plant

et al. 2017

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This study intends to check the effects of air pollutant prevention facilities in bituminous coal-fired power plants on N 2 O gas emission concentration. Bituminous coal-fired power plants install and operate air pollution prevention facilities to prevent air pollution. The exhaust gases generated by such coal-fired power plants generally pass through a flue gas denitrification facility for removal of nitrogen oxides, a dust collector for removal of suspended matter, and a flue gas desulfurization facility for removal of sulfur oxides and are emitted through a smokestack. To check the effects of prevention facilities on N 2 O emission concentrations, sampling is necessary at the front end and rear end of each prevention facility. Exhaust gases were collected from the front and rear ends of the flue gas denitrification facility (SCR), the rear end of the electric dust collector (EP), and the measurement hole on the smokestack to analyze the concentrations of the gases. According to the results, it was identified where N 2 O emission concentrations were affected by air pollution prevention facilities. In which air pollutant prevention facilities these differences occurred was analyzed. N 2 O emission concentration decreased after flue gases passed the flue gas desulfurization facility (FGD) in all three power plants. The phenomenon of reduction of N 2 O emission concentrations by bituminous coal-fired power plant FGD is judged attributable to the effect of CaCO 3 used in the FGD.

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“…Recently, density functional theory (DFT) calculations were applied to explain the micro‐mechanism of reactions . By studying SO 2 and CO 2 adsorption on pristine CaO and alkali‐metal‐doped CaO, Wang et al .…”

Section: Introductionmentioning

confidence: 99%

“…found CO 2 and SO 2 show strong adsorption, and the metal Cs is the preferred dopant for high sorption capacity. Wu et al . calculated transition states of different reactions to assure the complexity of the reactions occurring.…”

Section: Introductionmentioning

confidence: 99%

Mechanism of steam‐declined sulfation and steam‐enhanced carbonation by DFT calculations

et al. 2019

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Sulfur dioxide (SO2) and carbon dioxide (CO2) removals are of great significance for fossil fuel combustion, where they can be simultaneously captured by calcium‐based absorbents. Nevertheless, the CO2 uptake capacity declines with SO2 partial pressures. This paper aims at explaining the mechanisms of steam‐declined sulfation and steam‐enhanced carbonation by density functional theory calculations. CaO(001) surface is chosen as the absorbent, and the transition state is calculated to obtain the desorption barrier energy of the adsorbates. By analyzing the desorption of the adsorbate on pristine CaO(001) surface and the CaO(001) surface that has adsorbed other adsorbate, it can be concluded that SO2 adsorption inhibits CO2 adsorption since the barrier energy of CO2 desorption on SO2‐CaO(001) surface (24.15 kJ mol–1) is less than CO2 desorption on CaO(001) surface (129.52 kJ mol–1). By comparing the coadsorption energy of the two adsorbates with the sum of the adsorption energy of each adsorbate, it is practical that the H2O adsorption inhibits SO2 adsorption because the calculated coadsorption energy (−221.27 kJ mol–1) is larger than the sum of H2O adsorption energy (–100.00 kJ mol–1) and SO2 adsorption energy (−194.37 kJ mol–1). However, the calculated coadsorption energy of H2O and CO2 adsorption (−254.89 kJ mol–1) is less than the sum of CO2 adsorption energy (−144.23 kJ mol–1) and H2O adsorption energy (−100.00 kJ mol–1), indicating the promotion of CO2 adsorption. Steam in the adsorption process plays the roles of sulfation suppression and carbonation enhancement. © 2019 Society of Chemical Industry and John Wiley & Sons, Ltd.

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Effect of sulfation on the surface activity of CaO for N2O decomposition

Cited by 7 publications

References 39 publications

Mechanism of CO Oxidation on Cu₂O (111) Surface: A DFT and Microkinetic Study

Mechanism of CO Oxidation on Cu₂O (111) Surface: A DFT and Microkinetic Study

Study on the Variance of N₂O Concentration after Air Pollution Prevention Facility in Bituminous Coal-Firing Power Plant

Mechanism of steam‐declined sulfation and steam‐enhanced carbonation by DFT calculations

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Effect of sulfation on the surface activity of CaO for N2O decomposition

Cited by 7 publications

References 39 publications

Mechanism of CO Oxidation on Cu2O (111) Surface: A DFT and Microkinetic Study

Mechanism of CO Oxidation on Cu2O (111) Surface: A DFT and Microkinetic Study

Study on the Variance of N2O Concentration after Air Pollution Prevention Facility in Bituminous Coal-Firing Power Plant

Mechanism of steam‐declined sulfation and steam‐enhanced carbonation by DFT calculations

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Product

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Mechanism of CO Oxidation on Cu₂O (111) Surface: A DFT and Microkinetic Study

Mechanism of CO Oxidation on Cu₂O (111) Surface: A DFT and Microkinetic Study

Study on the Variance of N₂O Concentration after Air Pollution Prevention Facility in Bituminous Coal-Firing Power Plant