Author: Christopher Paolucci
Publisher:
ISBN:
Category :
Languages : en
Pages : 284
Book Description
Theoretical and Computational Modeling of the Selective Catalytic Reduction of NOx in Cu-SSZ-13 Zeolites
Author: Christopher Paolucci
Publisher:
ISBN:
Category :
Languages : en
Pages : 284
Book Description
Publisher:
ISBN:
Category :
Languages : en
Pages : 284
Book Description
Selective Catalytic Reduction of NOx
Author: Oliver Kröcher
Publisher: MDPI
ISBN: 3038973645
Category : Science
Languages : en
Pages : 281
Book Description
This book is a printed edition of the Special Issue "Selective Catalytic Reduction of NOx" that was published in Catalysts
Publisher: MDPI
ISBN: 3038973645
Category : Science
Languages : en
Pages : 281
Book Description
This book is a printed edition of the Special Issue "Selective Catalytic Reduction of NOx" that was published in Catalysts
Experimental and Kinetic Modeling Studies of Selective Catalytic Reduction of NOx with NH3 on Fe- and Cu-Zeolite Monolithic Catalysts
Author: Pranit Subhash Metkar
Publisher:
ISBN:
Category : Chemical engineering
Languages : en
Pages :
Book Description
The selective catalytic reduction (SCR) of NOx with NH3 is considered to be the most promising technique for the efficient reduction of highly detrimental NOx (to N2) emitted from diesel engine vehicles. Amongst the various catalysts available for SCR, Fe- and Cu-zeolite catalysts are found to be highly stable and efficient towards maximum NOx reduction over a wide temperature range. Cu-zeolites are more active at low temperatures ( 350 oC) while Fe-zeolites are more active at high temperatures ( 400 oC). We carried out a comprehensive experimental and kinetic modeling study of key SCR reactions on Fe- and Cu-zeolite catalysts and present a detailed understanding of mass transfer limitations and kinetics and mechanistic aspects of various SCR reactions on these catalysts. Experiments carried out on monolith catalysts having different washcoat loadings, washcoat thicknesses and lengths indicate the presence of washcoat (or pore) diffusion limitations at intermediate to high temperature range in all the SCR reactions. A detailed analysis of the effect of temperature on the transitions between various controlling regimes (kinetic, washcoat diffusion and external mass transfer) is presented. Agreement in the differential kinetics studies of NO oxidation and standard SCR (NO + O2 + NH3) reactions indicates NO oxidation is the rate determining step for standard SCR. A detailed kinetic model capturing key features of all the SCR reactions is developed. This model accurately predicts the experimentally observed NOx conversions over a wide temperature range and different feed conditions. Finally, a systematic study of various SCR reactions is carried out on a combined system of Fe- and Cu-zeolite monolithic catalysts to determine if a high NOx conversion could be sustained over a wider temperature range than with individual Fe- and Cu-zeolite catalysts. Amongst various configurations, a dual-layer catalyst with a thin Fe-zeolite layer on top of a thick Cu-zeolite layer resulted in a very high NOx removal efficiency over a broad temperature range of practical interest. The kinetic model accurately captures the experimental data with a combined system of Fe- and Cu-zeolite catalysts and provides further insights into the catalyst arrangements for maximum NOx reduction efficiency.
Publisher:
ISBN:
Category : Chemical engineering
Languages : en
Pages :
Book Description
The selective catalytic reduction (SCR) of NOx with NH3 is considered to be the most promising technique for the efficient reduction of highly detrimental NOx (to N2) emitted from diesel engine vehicles. Amongst the various catalysts available for SCR, Fe- and Cu-zeolite catalysts are found to be highly stable and efficient towards maximum NOx reduction over a wide temperature range. Cu-zeolites are more active at low temperatures ( 350 oC) while Fe-zeolites are more active at high temperatures ( 400 oC). We carried out a comprehensive experimental and kinetic modeling study of key SCR reactions on Fe- and Cu-zeolite catalysts and present a detailed understanding of mass transfer limitations and kinetics and mechanistic aspects of various SCR reactions on these catalysts. Experiments carried out on monolith catalysts having different washcoat loadings, washcoat thicknesses and lengths indicate the presence of washcoat (or pore) diffusion limitations at intermediate to high temperature range in all the SCR reactions. A detailed analysis of the effect of temperature on the transitions between various controlling regimes (kinetic, washcoat diffusion and external mass transfer) is presented. Agreement in the differential kinetics studies of NO oxidation and standard SCR (NO + O2 + NH3) reactions indicates NO oxidation is the rate determining step for standard SCR. A detailed kinetic model capturing key features of all the SCR reactions is developed. This model accurately predicts the experimentally observed NOx conversions over a wide temperature range and different feed conditions. Finally, a systematic study of various SCR reactions is carried out on a combined system of Fe- and Cu-zeolite monolithic catalysts to determine if a high NOx conversion could be sustained over a wider temperature range than with individual Fe- and Cu-zeolite catalysts. Amongst various configurations, a dual-layer catalyst with a thin Fe-zeolite layer on top of a thick Cu-zeolite layer resulted in a very high NOx removal efficiency over a broad temperature range of practical interest. The kinetic model accurately captures the experimental data with a combined system of Fe- and Cu-zeolite catalysts and provides further insights into the catalyst arrangements for maximum NOx reduction efficiency.
Computational Insights Into the Mechanism of the Selective Catalytic Reduction of NOx: Fe- Versus Cu-Exchanged Zeolite Catalysts
Author: Julian Rudolph
Publisher:
ISBN:
Category :
Languages : en
Pages :
Book Description
We computationally investigate the mechanism of the reduction half-cycle of the selective catalytic reduction of nitrogen oxides with ammonia. We compare both Fe- and Cu-exchanged zeolite catalysts and aim at exploring all accessible reaction pathways. From our calculations, a comprehensive picture emerges that unifies several previous mechanistic proposals. We find that both for Fe and for Cu catalysts different reaction pathways are feasible but some of the possible reaction pathways differ in these two cases. Our computational results provide a basis for the interpretation of in situ spectroscopic investigations that can possibly distinguish the different mechanistic pathways.
Publisher:
ISBN:
Category :
Languages : en
Pages :
Book Description
We computationally investigate the mechanism of the reduction half-cycle of the selective catalytic reduction of nitrogen oxides with ammonia. We compare both Fe- and Cu-exchanged zeolite catalysts and aim at exploring all accessible reaction pathways. From our calculations, a comprehensive picture emerges that unifies several previous mechanistic proposals. We find that both for Fe and for Cu catalysts different reaction pathways are feasible but some of the possible reaction pathways differ in these two cases. Our computational results provide a basis for the interpretation of in situ spectroscopic investigations that can possibly distinguish the different mechanistic pathways.
Atomic-level Insights Into the Hydrothermal Stability of CU/SSZ-13 SCR Catalysts for the Abatement of Diesel Vehicle Nox Emissions
Author: James Song
Publisher:
ISBN:
Category :
Languages : en
Pages :
Book Description
Publisher:
ISBN:
Category :
Languages : en
Pages :
Book Description
Selective Catalytic Reduction of NOx by NH3 (NH3-SCR) in Small Pore Cu-exchanged Chabazite (CHA) Catalysts
Author: Di Wang
Publisher:
ISBN:
Category : Chemical engineering
Languages : en
Pages :
Book Description
Nitrogen oxides, NOx (NO+NO2), are considered significant air pollutants. Selective catalytic reduction of NOx with NH3 (NH3-SCR) is a leading technology candidate for NOx emissions control for diesel engine vehicles. Recently, the Cu-exchanged chabazite framework type zeolite with small pores, such as SAPO-34 and SSZ-13, has received a great deal of attention due to exceptional hydrothermal durability and enhanced SCR activity. I have carried out a systematic study over both Cu-SAPO-34 and Cu-SSZ-13 catalysts to elucidate the reaction mechanisms, acid properties, Cu structures, active centers and deactivation modes. First, the intrinsic mechanism of the SCR reaction over a Cu-exchanged SAPO-34 catalyst at low temperature was studied by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), coupled with a mass spectrometer to measure inlet and outlet gas concentrations. The evolution of the surface intermediates, as well as the reactivity of NH3 with surface NOx species and NOx with surface NH3 species, was evaluated. Second, a series of SAPO-34 catalysts with various Cu loadings (ranging 0.7-3.0 wt%) was prepared by a solid state ion exchange method (SSIE). The acid properties as well as the Cu structures were characterized by XRD, NH3-TPD, UV-vis, DRIFTS and H2-TPR. Third, a SSIE method was developed to synthesize Cu-SSZ-13 catalysts with excellent NH3-SCR performance and durable hydrothermal stability. After the SSIE process, the SSZ framework structure and surface area was maintained. DRIFTS and NH3-TPD experiments provide evidence that Cu ions were successfully exchanged with Brønsted acid protons in the pores. Fourth, the hydrothermal stability of Cu-SAPO-34 and Cu-SSZ-13 was studied. Their different evolutions of zeolite framework, acidity and Cu structure during the hydrothermal aging were probed by XRD, DRIFTS and NH3-TPD. The results suggest that Cu-SAPO-34 is more resistant to hydrothermal aging in comparison to Cu-SSZ-13. Last, the SO2 poisoning effect over Cu-SAPO-34 catalyst was investigated by using in-situ DRIFTS combined with temperature programmed desorption (TPD) experiments. It was found that the low temperature deactivation mechanism involved the formation of ammonium sulfate species as well as the competitive adsorption SO2 with NOx.
Publisher:
ISBN:
Category : Chemical engineering
Languages : en
Pages :
Book Description
Nitrogen oxides, NOx (NO+NO2), are considered significant air pollutants. Selective catalytic reduction of NOx with NH3 (NH3-SCR) is a leading technology candidate for NOx emissions control for diesel engine vehicles. Recently, the Cu-exchanged chabazite framework type zeolite with small pores, such as SAPO-34 and SSZ-13, has received a great deal of attention due to exceptional hydrothermal durability and enhanced SCR activity. I have carried out a systematic study over both Cu-SAPO-34 and Cu-SSZ-13 catalysts to elucidate the reaction mechanisms, acid properties, Cu structures, active centers and deactivation modes. First, the intrinsic mechanism of the SCR reaction over a Cu-exchanged SAPO-34 catalyst at low temperature was studied by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), coupled with a mass spectrometer to measure inlet and outlet gas concentrations. The evolution of the surface intermediates, as well as the reactivity of NH3 with surface NOx species and NOx with surface NH3 species, was evaluated. Second, a series of SAPO-34 catalysts with various Cu loadings (ranging 0.7-3.0 wt%) was prepared by a solid state ion exchange method (SSIE). The acid properties as well as the Cu structures were characterized by XRD, NH3-TPD, UV-vis, DRIFTS and H2-TPR. Third, a SSIE method was developed to synthesize Cu-SSZ-13 catalysts with excellent NH3-SCR performance and durable hydrothermal stability. After the SSIE process, the SSZ framework structure and surface area was maintained. DRIFTS and NH3-TPD experiments provide evidence that Cu ions were successfully exchanged with Brønsted acid protons in the pores. Fourth, the hydrothermal stability of Cu-SAPO-34 and Cu-SSZ-13 was studied. Their different evolutions of zeolite framework, acidity and Cu structure during the hydrothermal aging were probed by XRD, DRIFTS and NH3-TPD. The results suggest that Cu-SAPO-34 is more resistant to hydrothermal aging in comparison to Cu-SSZ-13. Last, the SO2 poisoning effect over Cu-SAPO-34 catalyst was investigated by using in-situ DRIFTS combined with temperature programmed desorption (TPD) experiments. It was found that the low temperature deactivation mechanism involved the formation of ammonium sulfate species as well as the competitive adsorption SO2 with NOx.
New and Future Developments in Catalysis
Author: Zdenek Sobalik
Publisher: Elsevier Inc. Chapters
ISBN: 0128081198
Category : Science
Languages : en
Pages : 68
Book Description
Publisher: Elsevier Inc. Chapters
ISBN: 0128081198
Category : Science
Languages : en
Pages : 68
Book Description
Selective catalytic reduction of NOx with NH3
Author: Hanna Sjövall
Publisher:
ISBN: 9789173853453
Category :
Languages : en
Pages : 68
Book Description
Publisher:
ISBN: 9789173853453
Category :
Languages : en
Pages : 68
Book Description
Theoretical Study of the Electronic Structure and Reactions Involving Oxygen-Bridged Cu-Pairs in Zeolite Catalysts for Lean Nitric Oxide Abatement
Author:
Publisher:
ISBN:
Category :
Languages : en
Pages :
Book Description
Publisher:
ISBN:
Category :
Languages : en
Pages :
Book Description
Cu-ZSM-5 Zeolite Catalysts for the Selective Catalytic Reduction of NOx
Author: Jan Connerton
Publisher:
ISBN:
Category :
Languages : en
Pages :
Book Description
Publisher:
ISBN:
Category :
Languages : en
Pages :
Book Description