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149-188

149-188

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11/28/2013

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*
Corresponding author (Z. Ziaka). Tel/Fax: +30-2310-275473 E-mail addresses:bookeng@hotmail.com,z.ziaka@ihu.edu.gr.
2013. American Transactions onEngineering & Applied Sciences. Volume 2 No. 2 ISSN 2229-1652 eISSN 2229-1660Online Available athttp://TuEngr.com/ATEAS/V02/149-188.pdf  
 
149
 
American Transactions onEngineering & Applied Sciences
http://TuEngr.com/ATEAS 
Catalytic
 
Decomposition
 
of 
 
N
2
O:
 
Best 
 
 Achievable
 
Methods
 
and
 
Processes
 
Paschalia Taniou
a
, Zoe Ziaka
a*
, Savvas Vasileiadis
a
 
a
Department of Science and Technology, Laboratory of Environmental Catalysis,
 
Hellenic OpenUniversity, Patras, GREECE.
A R T I C L E I N F O
 
A B S T RA C T
Article history
:Received February 01, 2013Received in revised formFebruary 26, 2013Accepted March 07, 2013Available onlineMarch 11, 2013
Keywords
: N
2
O decomposition;split N
2
O;catalytic zeolite systems;cobalt spinels;Rh catalytic systems;Cu catalytic systems;membrane N
2
O separation.
In the current review paper, the N
2
O direct decompositionwas investigated over a series of different catalytic systems,containing metals, zeolites, cobalt spinels. The N
2
O split via catalysisand the use of membrane systems in the separa
 
tion to molecules N
2
 and O
2
were studied, too. Decomposition of N
2
O has been studied inthe temperature rate of 673 to 873 K over supported catalysts of chemical elements: Pd, Rh, Ru, Ni, Pt, Zn, Fe, Cu, Ir, over 
γ
- Al
2
O
3
 showing their best catalytic activity. M-zeolites, (M = Cu, Fe, Co,etc.) supported on perovskite or precious metals such as Pd, Rhzeolites and dominant iron and copper catalytic structures such asZSM-5, MFI, BEA, BETA investigated in the temperature rate of 583to 775 K with best catalytic activity. Iron zeolites are more prevalentat high concentrations showing good catalytic behavior only at hightemperatures. The spinel catalyst Zn
0.36
Co
0.64
Co
2
O
4
and Rh/Mullitecatalyst offer up to complete N
2
O conversion.
2013 Am. Trans.
 
Eng. Appl. Sci.
 
1.
 
Introduction
 
It is well known that nitrous oxide is considered a dangerous environmental pollutant becauseit contributes to the destruction of stratospheric ozone and simultaneously is also considered as a
2013 American Transactions on Engineering & Applied Sciences.
 
150
Paschalia Taniou, Zoe Ziaka, and Savvas Vasileiadis
greenhouse gas. The concentration of N
2
O in the atmosphere increases every year up to0.2–0.3%, and this increase is caused mainly by anthropogenic activities. More specific, chemical processes related to the production and use of nitric acid and fluidized bed combustion are the twomain nitrous oxide sources, and their contribution to the total nitrous oxide emissions amounts upto 20%. Minimization of N
2
O emission can be accomplished mainly by two ways, either bylowering the formation of N
2
O or after treatment where catalysis introduces the N
2
O abatement bythe direct decomposition into nitrogen and oxygen. Metal such as transition metal oxides, zeolitesand noble metals, especially rhodium, dispersed on oxide supports exhibit catalytic activity in N
2
Odecomposition.[1]  Nitrous oxide (N
2
O), for many years has not received the attention of scientific interest. But, inrecent years, due to the significant impact of greenhouse gases in the atmosphere and the increasingannual concentration a research activity has started, which involves various processes andtechnologies of reduction of it and splitting into harmless molecules, N
2
and O
2
.A well understandable picture of the global nitrogen cycle is shown in Figure 1. (1) urbanareas: NO
x
is produced from high-temperature combustion. (2) Biomass burning: NO
x
, NH
3
, and N
2
O are produced from combustion of plant materials. (3) Agriculture: nitrogen is fixed throughfertilizer manufacturing and the planting of nitrogen-fixing crops. Denitrification produces N
2
and N
2
O. NH
3
is produced from fertilizer use and livestock excreta. (4) Natural fluxes: nitrogen fixingmicrobes in soil and sea water supply plants with usable nitrogen. Denitrification releases N
2
and N
2
O to atmosphere. (5) Wet and dry deposition: Nitrate and ammonia are removed from theatmosphere to both land and sea. (6) Lightning: NO
x
is produced via high-temperature reaction of  N
2
and O
2
. [2]The following mechanisms is proposed for the direct N
2
O decomposition:(a) N
2
O + (*)
Æ
N
2
+ *O N
2
O + *O
Æ
N
2
+ O*OO*O
Æ
O
2
+ (*)(b) 2N
2
O + 2(*)
Æ
2N
2
+ 2*O2*O
Æ
O
2
+ 2(*)(c) N
2
O + (*)
Æ
N
2
+ *O
 
*
Corresponding author (Z. Ziaka). Tel/Fax: +30-2310-275473 E-mail addresses:bookeng@hotmail.com,z.ziaka@ihu.edu.gr.
2013. American Transactions onEngineering & Applied Sciences. Volume 2 No. 2 ISSN 2229-1652 eISSN 2229-1660Online Available athttp://TuEngr.com/ATEAS/V02/149-188.pdf  
 
151
  N
2
O + *O
Æ
N
2
+ *O
2
  N
2
O + *O
2
 
Æ
N
2
+ *O
3
 *O3
Æ
*O +O
2
 
Figure 1:
Nitrogen cycle [2].In mechanism (b) (Langmuir–Hinshelwood mechanism), the migration of oxygen from oneactive site (*) followed by recombination with another oxidized site is the rate-determining step.This reaction mechanism requires the active participation of, at least, two iron centers that are notnecessarily located in adjacent positions. In mechanisms (a) and (c) (Eley–Rideal mechanisms),  N
2
O decomposition and oxygen evolution occur at the same isolated sites (*) after successivecollisions between N
2
O with (*) and *O for (a), and with (*), *O, and *O
2
for (c). The proposedabove mechanisms are all in agreement with transient response experiments, showing that N
2
 appears before O
2
upon direct N
2
O decomposition pulses in the 773 to 848 K temperature range.This is happens because in all cases the global decomposition reaction is limited by the reactionssteps leading to gas O
2
. More specific, recently accurate temporal analysis of products stronglyimplies that mechanism (a) is the most likely. On the other hand, from the point of view of theoxygen species formed on iron active sites (*), the three mechanisms are associated with

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