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Contents lists available at ScienceDirect
Applied Catalysis A: General
j ournal homepage : www.elsevier .com/ locate /apcata
Critical evaluation ofthe role ofthe distribution ofAl atoms in theframework for the activity ofmetallo-zeolites in redox N2O/NOxreactions
Zdenek Sobalik, Petr Sazama,Jiri Dedecek, BlankaWichterlov
J. Heyrovsky Institute of Physical Chemistry, Academy of Sciences of the Czech Republic, CZ-182 23 Prague 8, Czech Republic
a r t i c l e i n f o
Article history:Received 28 February 2013
Received in revised form 6 June 2013
Accepted 16 July 2013
Available online xxx
Keywords:
Cu-zeolite
Co-zeolite
Fe-zeolite
SCR-NOx
NO decomposition
N2O decomposition
Al distribution in theframework
Al pairs in zeolites
ZSM-5
Thebeta zeolite
a b s t r a c t
Both the laboratory synthesized zeoliteswith tailoreddistributionofframeworkAlatoms andcommercial
ZSM-5 zeolites ofvarious proveniences were investigated in a broad region ofSi/Al ratio with respect to
the distribution ofAl atoms in the framework. The analysis of the distribution of framework Al atoms
was done by using strictly defined conditions ofCo(II) ion exchange and UVVis, 27Al and 29Si (CP) MAS
NMRexperiments. Evidence has been found that the distribution offramework Al atoms in ZSM-5, and
in Si-rich zeolites in general, is not random and is not controlled by statistics, but occurs between the
most populated Al pairs (AlSiSiAl sequences in 6MRs) and single far distant Al atoms (AlSin>2Al
sequences) located in different rings. Depending on the type of Si- and Al-reactants and presence of
TPA+/Na+ ingels, a broaddistribution ofAl atoms(from5 to 85%ofAl atoms inAl pairs) for Si/Al 1220can
be achieved. At Si/Al >20, the population ofAl pairs decreases, but 90% ofsingle Al atoms can be obtained
in the whole range ofSi/Al compositions. The local negative charge ofthe framework governed by the
distribution of framework Al atoms inevitably controls the structure of the counter metal ion species,
which is reflected in the catalytic properties ofmetallo-zeolites in redox reactions requiring different
types ofcounter ion species. A high population ofAl pairs in the framework is required for stabilization
ofdivalentbareCu(II),Co(II)and Fe(II) ionsboth inZSM-5and thebetazeolite, representing the active sites
forC10H22-SCR-NOx,CH4-andC3H8-SCR-NOx, and forN2Odecomposition, respectively. Incontrast, singleAl atoms charge-balance monovalent cations, metal-oxo or bridged metal-oxo(hydroxo) species, the
active sites forNOdecomposition (Cu(I) in ZSM-5and BEA*), forNH3-SCR-NOx toN2 andNO-NO2 reaction
(Fe(III)-oxo species in ZSM-5) and C3H8-SCR-NOx/H2O (Co(II)-oxo in BEA*) in the presence of a large
excess ofwater existing in real exhaust gases. Itis concluded that control ofthe distribution ofAl atoms
in the framework byhydrothermal synthesis ofSi-rich zeolites could achieve the high concentration ofan
appropriate active structure ofcountermetal-ion species required for a specified reaction andconditions.
Thus, in addition to the usually reported total concentration ofAl atoms, the distribution ofAl atoms in
the framework, i.e. the local negative framework charge, is a parameterwhich should be included in the
characteristics ofSi-rich zeolites.
2013 The Authors. Published by Elsevier B.V. All rights reserved.
1. Introduction
Stabilization of thecounter ionspecies asprotons and/ormono-
andpolyvalentcations,and theirmetal-oxospeciesinside adefined
microporevolumeby thenegative charge of the crystallinealumi-
nosilicate framework predeterminesH- andmetallo-zeolites to act
This is an open-access articledistributed under the terms of theCreative Com-
mons Attribution-NonCommercial-No Derivative Works License, which permits
non-commercial use, distribution, and reproduction in anymedium, provided the
original authorand source arecredited. Corresponding author.
E-mail address: [email protected](Z. Sobalik).
as efficient and highly selective catalysts for oil and hydrocarbon
processing, forselectivehydrocarbonoxidation, thedecompositionandreduction of nitrogen oxides in environmentprotection andin
fine chemicals synthesis. Si-rich zeolites of ZSM-5, ferrierite, mor-
denite and the beta zeolite structures (MFI, FER, MORand BEA*,
respectively) have attracted great attention, because of the low
aluminum concentration in the framework (Si/Al> 8) leading to
strong acidity of the protons (see, e.g. Ref. [1]) and unusual redox
and catalytic behavior of transition metal ion species (see, e.g.
Refs. [213]), as well as shape selective effects of their microp-
ores.
Theoverall concentration of Al atoms in the frameworkand the
related concentration of protons and/or cations and oxo-cations
0926-860X/$ seefrontmatter 2013 The Authors. Published by Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.apcata.2013.07.033
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Fig. 1. Effect of thelocal arrangement of Al atoms in theframework of ZSM-5 on theexchangeof Co(II)-complexes andbonding of Co(II)ions in dehydrated zeolites.
Alunpair= 2x[Co(II)(H2O)6)]2+
max 2xCo(II)bare (3)
[AlFR] = [Alpair] + [Alunpair] + [Alsingle] (4)
where [Co(II)(H2O)6]2+
max is the Co(II) ion-exchange capacity of
[Co(II)(H2O)6]2+ ions, Co(II)bare is the concentration of bare Co(II)
in dehydrated zeolites, Co(II),, are concentrations of Co(II) ions
in,and cationicsites, [Alpair]istheconcentrationofAlatomsin
theAlSiSiAlsequencein one(6MR)ringof cationicsite, [Alunpair]is the concentration of close Al atoms located in different rings,
[Alsingle] is the concentration of single far-distant Al atoms, and
[AlFR] is the total concentration of Al in the framework.
For ZSM-5 zeolites with framework Si/Al 1240 compositions
analyzedso far, theconcentration of bare Co(II) ions in dehydrated
zeolites was equal (within 5% error) to the [Co(II)(H2O)6]2+ ion-
exchange capacity. Similarly, the concentration of Alunpair, where
Co-oxospecies were observed in theUVspectra, didnot exceed3%
of total Al present in the zeolite.
To obtain a correct analysis of the Al distribution in the frame-
work, the exclusive exchange of [Co(II)(H2O)6]2+ complexes into a
zeolite without their hydrolysis must be guaranteed. Based on the
extensiveexperimentalexperience[45] andseeRef.[37], thiscould
be satisfied by carrying out the ion exchange from dilute aque-ous solutions 0.05M of Co(NO3)2 under mildly acidic conditions
(6> pH> 5)at RT intotheNa-formofthezeolite. The accuracyof the
estimation of the concentration of [Co(II)(H2O)6]2+ complexes in
hydrated zeolites depends on Co concentration. It varies between
2% for Al rich (Si/Al< 10) zeolites with large portion of Al pairs
(Co/Al> 0.3) and 1015% for zeolites with low concentration of Al
pairs (Si/Al 2540, Co/Al< 0.25).
The exclusive presence of [Co(II)(H2O)6]2+ complexes in the
solution and inside the Co-exchanged zeolite can be monitored
by Vis spectroscopy by a typical spectrum of the strictly octahe-
dral Co(II) complex shown in Fig. 2. All conceivable changes in
the environmentof theCo(II) ionthe octahedral hexaquo-complex
(e.g. formation of [Co(II)(H2O)5X]+ or Co(II) oligomeric species)
would result in breaking down of the symmetry of this complex
reflected in the formation of new spectroscopic species [44,46].
The change of the spectrum of the Co(II)-exchanged zeolite due
to the presence of an additional Co(II) complex to [Co(II)(H2O)6]2+,
i.e. [Co(II)(H2O)5OH]+, is demonstrated in Fig. 2, where the spec-
tra of Co-ZSM-5 prepared by the ion exchange with Co(II) nitrate
and Co(II) acetate are compared. The Co(II) exchange into the Na-
zeolite guarantees attainment of themaximumexchange leveldue
to faster ion exchange into the Na- compared to H-zeolites. Na-
formof azeolitealsoprevents formationofanynitrogen-containingCo(II)complexesthatcouldbeformedduringtheCo(II)-exchange, if
itwouldbedonewithNH4-zeolites.Reproducibilityof thedetermi-
nationof theexchangecapacityof [Co(II)(H2O)6]2+ ionswaswithin
5 rel.%, i.e. within the error of chemical analysis, as revealed from
seriesof experiments done with Na-ZSM-5 samples of Si/Al 12 and
22.
Fig. 2. Normalized Visspectra of theas prepared hydrated Co-ZSM-5, Si/Al 14.1.
Sample with Co/Al 0.41 prepared by equilibration with Co(NO3)2 at RT (), and
Co/Al 0.54 prepared by ionexchange from Co(acetate)2 at80
C (- - -).
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Fig. 3. Concentration of Al atoms in Al pairs in commercial ZSM-5 zeolites (), and
statistical prediction of their maximum () and minimum (- - -) concentration in
6MRs according to Ref. [24].
Theanalysisof the distributionof frameworkAlatoms inSi-rich
zeolitesconcludedoccurrenceof twodominantSiAlarrangements
intheframeworkofZSM-5zeolites,andin Si-richzeolitesgenerally,which are represented by (i) the AlSiSiAl sequences (Al pairs)
located in 6MRs enabling to balance bare divalent cations in dehy-
dratedzeolites,and (ii) the fardistant single Al atoms inAlSin>2Al
sequences located in different rings not providing coordination of
a divalent cation, butwith potential to chargebalancemonovalent
species.
3. ZSM-5 zeolite samples
ZSM-5 zeolites analyzed here included products of several
industrial producers, i.e. Conteca, ALSI-PENTA, Tosoh, SdChemie
and PQ Corporation with Si/Al ranging from 12 to 45. The identity
and crystallinity of these samples was generally checked by XRD,
and their pore volumes corresponded to well-developed ZSM-5structures. Chemical analysis and the 27Aland 29SiMASNMRspec-
traindicatedhighproportionof Td-coordinatedAl intheframework
and 12), the AlSiSiAl
sequences(Alpairs) locatedin 6MRs,andsinglefar-distantAlatoms
in AlSin>2Al sequences. The concentration of close Al atoms in
different rings (Alunpair) was below 5%of total Al.
4. Distribution of the framework Al atoms in commercial
ZSM-5
The concentrations of Al atoms in Al pairs (AlSiSiAl
sequences in 6MRs) found in commercial samples with differ-
ent Si/Al ratios are given in Fig. 3. Obviously, a general trend in
Fig. 4. Variability of the concentration of Al atoms in Al pairs using hydrothermal
synthesesaccording to Ref. [22] (), Ref. [21] (), Ref. [33] () and Ref. [45] ().
decreasing relative concentrations of Al atoms accommodated in
Al pairs with decreasing total Al concentration in the framework
is observed, with a sharp decrease in the range of Si/Al 1220.
Nevertheless, this tendency displays large differences in the actualconcentrations of Al atoms in Al pairs for samples with close Si/Al
composition up to ca 20 rel.%, i.e. highly exceeding the accuracy
of determination of the distribution of frameworkAl atoms (5%).
Thepopulations of Al pairs predictedby using a simplistic statisti-
cal approach arealso summarized in Fig. 3 dependingon Si/Al. The
results of statisticalcalculationsofRiceet al. [24] areshownby lines
depicting the concentration of Al atoms in the Al pairs under the
conditions of applicationof the Lowensteinrule and therestriction
for location of Al pairs only in 6MRs. Thus the lines given in Fig. 3
excluded sites with two Al atoms in 5MRrings, in agreementwith
our 29Si MAS NMRobservation revealing the absence of AlSiAl
sequences in ZSM-5 of Si/Al >12. The clear discrepancy between
the experimental results and the statistical calculations should be
regarded as being a result of direct practical relevance showingthat the concentrations of Al pairs for the individual commercial
samples donot followtheexpected simplestatistics. Dramatic dif-
ferences between the distributions of Al atoms found for samples
with close Al content in the framework represent additional sup-
port for thepreviousconclusion on thenon-randomdistributionof
Al atoms in ZSM-5zeolites not controlled by statistical rules. These
differences observed for commercial ZSM-5 indicate that the Si/Al
compositionisnotthesingleparametercontrollingthedistribution
of Al atoms.
5. Variability in the distribution of framework Al atoms in
ZSM-5 caused by hydrothermal synthesis conditions
Hydrothermal laboratory syntheses of ZSM-5 zeolites carriedout in the presenceofa template (TPAOH)andusingvariousSi-and
Al-reactants,Si/Al gelcompositions,andin thepresence/absenceof
Na+ ions (details reported in Refs. [2022,33,34,45]) led to a high
variability in the distribution of Al atoms in the framework over
a wide range of Si/Al compositions (Fig. 4). For Si/Al 1215 in the
products the concentrations of Al atoms in Al pairs could be tuned
from5 to 85% by changing the composition of the reactants.While
a highly predominant concentration of single Al atoms could be
obtained ina widerange ofSi/Al from12to 45, the chanceto incor-
porate Al pairs obviouslydecreaseswithdecreasing concentration
of frameworkAl atoms.
Fig. 5 depicts sets of hydrothermal syntheses carried out with
various reactants (Al chloride vs. Al nitrate; TEOS vs. Na-silicate
vs. Si-Al precursor) under the same (volume, T, Si/TPAOH 2.8)
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Fig. 5. Effect of Si/Al on the concentration of Al atoms in Al pairs in ZSM-5 zeolite
for hydrothermal syntheses using: Al chloride+ TEOS (), Si-Al precursor (), Al
nitrate +TEOS (), Al nitrate+ Na silicate (); according to Refs. [33,32].
conditions of hydrothermal synthesis. It was shown that the use
of Al nitrate and Na-silicate in the gel strongly supports the
incorporation of single Al atoms into the framework, while theSiAl precursor and AlCl3/TEOS yield a higher population of Al
pairs. Moreover, while the gel containing the SiAl precursor or
AlCl3/TEOS exhibited a decrease in the concentration of Al pairs
with increasing Si/Al ratio, quite the opposite trend was obtained
withAlCl3/TEOS gels. A markedeffectof Si/Al was not observed for
ZSM-5 products with low population of Al pairs and high popula-
tion of single Al atoms (90% of total Al). These findings strongly
support the suggestion of the decisive role of the type of reactants
on the distribution of Al atoms in the framework of ZSM-5 zeo-
lites, and further contradict the assumption about the random or
statistical distributionof frameworkAl atoms.
Analysisof themechanismbehind thehydrothermalZSM-5syn-
thesis leading to incorporation of Al pairs vs. single Al atoms in
the framework and understanding of the function of the individ-ual reactants are beyond the scope of this paper. We have already
suggestedthat the polarizationof TPA+ by anions andthe presence
of Na+ ions play a decisive role in the arrangement of the Al atoms
in SiAl sequences during the first stages of the interactions in the
gel. For details on the 29Si, 27Al and 13C MAS NMR study of the
gel composition and corresponding distributionof Al atoms in the
framework of ZSM-5 products, the reader is referred to the recent
paper of Dedecek et al. [33].
6. Impact of the distribution of framework Al atoms on
catalytic NOx processes over metallo-zeolites
Obviously, the structure of the resulting counter-ion species in
Si-rich zeolites obtained by ion exchange (in both aqueous andgaseous (CVD) environment) is controlled by both the counter
parts, i.e. the type of metal ion complex and the local nega-
tive charges occurring in the framework and governed by the
presence of Al pairs and single Al atoms. While the exchanged
[M(II)(H2O)6]2+ complexes in zeolites are predominantly balanced
by Al pairs, the negative charge of single Al atoms is sufficient for
monovalent [M(II)(H2O)5X]+ entities. After zeolite dehydration,
the Al pairs in 6MRs strongly stabilize bare divalent cations coor-
dinated to the framework oxygen atoms (see Fig. 1). At the same
time,monovalent species adjacent to singleAl atoms (monovalent
cationsormetal-oxo(hydroxo) ions), or bridgedmetal-oxospecies,
charge-balanced by two single Al atoms in different rings, can be
formed. An analogous (but more complex) situation, necessarily
considering the total positive charge of the metal complex, exists
Fig. 6. Effect of Cu loading in Cu-ZSM-5 on TOF in C10H22-SCR-NO under water
presence at 250C and inNOdecomposition at 400 C (seeRef. [51]).
for the location and charge balance of oxo(hydroxo) complexes of
trivalent cations.
Theobjective of this paper is nota detailedanalysis of thestruc-ture of various counter species, but rather to evaluate the effect
of the distribution of Al atoms in the framework on the activity of
the counter-ion species in Si-rich zeolites in redox reactions stud-
ied in our laboratory. This effect is outlined on the Cu-, Fe- and
Co-zeolites of ZSM-5 and beta structures with various distribu-
tions of Al atoms in the framework, and their activity in NO and
N2O decomposition, in oxidation of NO to NO2 and SCR-NOx by
methane, propane, decane or ammonia,moreover, in the presence
and absence ofwater vapor in the feed.
6.1. Cu-ZSM-5 and Cu-BEA*
While the ion exchange from aqueous Cu(II) nitrate solutions
preferablyoccurs through [Cu(II)(H2O)6]2+, theionexchange usingCu acetate solutions also includes [Cu(II)(H2O)5X
]+ complexes,
exchanged particularly intothehighly-loadedCu-ZSM-5. First, and
preferably at low loadings, the Cu(II) ions adjacent to the Al pairs
in 6MRs of cationic sites are exchanged, followed by introduc-
tion of [Cu(II)X]+ complexes charge-balanced mostly by single
Al atoms. In the dehydrated samples, the bare Cu(II) ions (orig-
inated from [Cu(II)(H2O)6]2+) are not easily reduced compared
to [Cu(II)(H2O)5X]+ transformed into [Cu(II)OH]+ or dinuclear
[Cu(II)-O-Cu(II)]2+ bothreadilyreduced toCu(I),whichsurviveeven
in oxygen atmosphere at elevated temperatures [3,4,47]. These
conclusions are based on the blue-shift in the UV-Vis spectrum of
theCu(II) aquocomplexes,and characteristic luminescencespectra
of bare Cu(I) ions, IR spectra of Cu(II)NO complexes [48,49], and
their redox properties in dehydrated Cu-zeolites [49,50].The TOF per Cu atom of NO decomposition over Cu-ZSM-5
clearly increaseswithincreasingCu/Alconcentrations (asobserved
in many laboratories) similar to the increasing population of Cu
species adjacent to single Al atoms (Fig. 6, data from Refs. [4,51]).
Accordingly, the active sites in NO decomposition represent the
generallyacceptedCu(I) ions,which areadjacenttosingleAlatoms,
more populated in the highly loaded Cu-zeolites. Similar high
activity inNOdecomposition (inTOF perCu)of the Cu ions charge-
balanced by single Al atoms and reflected in the shift of the high
energy edgeof the Cu(II) Vis band in the spectrumof hydrated Cu-
zeolite was observed and is depicted in Fig. 7 (data given in Ref.
[52]).
In contrast, the rateof the C10H22-SCR-NOx/H2O reaction in the
presence of water (12%) over Cu-ZSM-5 sharply decreases with
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Fig. 7. The effect of the position of high energy edge of the Cu(II) Vis band ofmax-
imum loaded hydrated Cu-BEA* samples prepared from different parents on the
conversion of NO perCu forNO decomposition (see Ref. [52]).
Fig. 8. Effect of Co loading on the yield of N2 in C3H8-SCR-NOx over Co-BEA-I ()
with prevailing concentration of single Al atoms (Si/Al 15.6, Alsingle0.59mmolg1,
61%), and Co-BEA-II () with lower concentration of single Al atoms (Si/Al 11.7,
Alsingle 0.41mmol g1, 34%). Maximum concentrations of bare Co(II) ions balanced
by Al pairs are indicated forCo-BEA zeolites by arrows. Data taken from Ref. [60].
Cu-loading (Fig. 6, for details see Ref. [51]). This indicates that, in
this reaction, the most active sites represent the Cu(II) ions bal-
anced by Al pairs. With the SCR-NOx reaction the redox process
requires divalent Cu(II) as the active site with participation of the
Cu(II)/Cu(I) redox cycle. However, the presence of water vapor is
knowntobedetrimental for the open coordination sphereof Cu(II)
ions balancedby Al pairs. Nevertheless, in this reaction carried outat250 C a strong adsorption of predominantly of olefinic products
of decane cracking and of NO2 on Cu(II) occurs, preventing water
adsorption.
6.2. Fe-ZSM-5
Fe ion exchange into ZSM-5 is very complex. In aqueous solu-
tions of Fe salts of both Fe(II) and Fe(III) ions substantial hydrolysis
takesplace [37]. In the procedureusing chemicalvapor deposition
from FeCl3, the FeCl2+ and FeCl2+ species are exchanged with fol-
lowing their hydrolysis. Various procedures employed for Fe ion
exchange led in dehydrated Fe-ZSM-5 (even in oxidizing atmo-
sphere) at lowFe loadings(Fe/Al
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[30] J. Dedecek, D. Kaucky, B. Wichterlova, O. Gonsiorova, Phys. Chem. Chem. Phys.4 (2002)54065413.
[31] O.H.Han,C.S.Kim,S.B. Hong, Angew. Chem. Int. Ed. 41 (2002) 469472.[32] O.Bortnovsky,O. Tokarova,B.Wichterlova,J. Dedecek,Z. Sobalik,O. Gonsiorova,
V. Balgova, (PatentWO2011095140).[33] J. Dedecek, V. Balgova, V. Pashkova, P. Klein, B. Wichterlova, Chem. Mater. 24
(2012)32313239.[34] V. Gabova, J. Dedecek, J. Cejka, Chem. Commun. (2003) 11961197.[35] P. Sazama, J. Dedecek, V. Gabova, B. Wichterlova, G. Spoto, S. Bordiga, J. Catal.
254 (2008) 180189.[36] Z. Sobalik, J. Novakova,J. Dedecek, N.K. Sathu,E. Tabor,P. Sazama, P. Stastny, B.
Wichterlova, Micropor.Mesopor.Mater. 146 (2011) 172183.[37] C.F. Baes, R.E. Mesmer, TheHydrolysis of Cations,Wiley,New York, 1976.[38] N. Katada, T. Kanai, M. Niwa, Micropor.Mesopor. Mater. 75 (2004) 6167.[39] T.I. Koranyi, J.B. Nagy, J. Phys. Chem. B 109 (2005) 1579115797.[40] S. Kuriyavar, O. Bortnovsky, Z. Tvaruzkova, Z. Sobalik, Collect. Czech. Chem.
Commun. 66 (2001) 685692.[41] J. Dedecek,D. Kaucky, B.Wichterlova,Micropor.Mesopor.Mater. 3536 (2000)
483494.[42] J. Dedecek, J. Cejka, M. Oberlinger, S. Ernst, Stud. Surf. Sci. Catal. 142 (2002)
2330.[43] L. Benco, T. Bucko, J. Hafner, H. Toulhoat, J. Phys. Chem. B 109 (2005)
2036120369.[44] J. Dedecek, L. Capek, D. Kaucky, Z. Sobalik, B. Wichterlova, J. Catal. 211 (2002)
198207.
[45] V.Gabova, PhDThesis,J. HeyrovskyInstitute of Physical Chemistryof theASCR(2004).
[46] D. Kaucky, J.I. Dedecek, B. Wichterlova, Micropor. Mesopor. Mater. 31 (1999)7587.
[47] Y. Kuroda, M. Iwamoto, Top. Catal. 28 (2004) 111118.[48] J. Dedecek, B. Wichterlova, J. Phys. Chem. B 101 (1997) 1023310240.[49] J. Dedecek, Z. Sobalik, Z. Tvaruzkova, D. Kaucky, B. Wichterlova, J. Phys. Chem.
99 (1995)1632716337.[50] R. Bulanek, B.Wichterlova,Z. Sobalik, J. Tichy,Appl.Catal. B-Environ. 31 (2001)
1325.[51] J. Dedecek, L. Capek, B. Wichterlova, Appl. Catal. A-Gen. 307 (2006) 156164.
[52] J. Dedecek, O. Bortnovsky, A. Vondrova, B. Wichterlova, J. Catal. 200 (2001)160170.
[53] P. Sazama, N.K. Sathu, E. Tabor, B. Wichterlova, S. Sklenak, Z. Sobalik, J. Catal.299 (2013) 188203.
[54] K. Jisa, J. Novakova, M. Schwarze, A. Vondrova, S. Sklenak, Z. Sobalik, J. Catal.262(2009) 2734.
[55] E. Tabor, K. Zaveta, N.K. Sathu, A. Vondrova, P. Sazama, Z. Sobalik, Catal. Today175 (2011) 238244.
[56] D.Kaucky,A.Vondrova,J. Dedecek,B. Wichterlova,J. Catal.194 (2000) 318329.[57] J.N. Armor, Catal. Today 26 (1995) 147158.[58] A.W. Aylor, L.J. Lobree, J.A. Reimer, A.T. Bell, Stud. Surf. Sci. Catal. 101 (1996)
661670.[59] L. Capek, J. Dedecek, B.Wichterlova, J. Catal. 227 (2004) 352366.[60] L. Capek, J. Dedecek, P. Sazama, B.Wichterlova, J. Catal. 272 (2010) 4454.
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