Introduction
The synthesis and properties of highly ordered meso-
porous materials M41S were reported by the Mobil
scientists fifteen years ago [1, 2]. The silica based
MCM-41 as a member of this family of the materials
attracted most attention due to its hexagonal array of
uniform pores, the high surface area and high total
pore volume. Although the structural properties of
these mesoporous solids as well as various routes of
their synthesis were extensively investigated over the
last years, the processes inside the pores at subse-
quent stages of the preparation procedure are still un-
der discussion. The surfactant transformations against
the temperature during calcination are well recog-
nized up to ~250°C. Above this temperature in the ox-
idizing atmosphere the chemical species present in-
side pores are transformed into carbon dioxide and
water. The thermal decomposition of the surfactant
template (CTAB) was studied in detail using the TPD
technique [3–6]. High temperature treatment of as-
synthesized MCM-41 changes additionally the con-
centration of the surface hydroxyls, which decreases
upon calcination [7, 8]. The most commonly method
used to remove the template is the calcination in air.
After calcination on the silica surface remain hardly
removable carbon deposits or coke [9–11].
The mechanism of the surfactant decomposition
during calcination has a step-character as described
by Kleitz et al. [12, 13]. They suggested that below
250°C 46% of the template is removed by hexadecene
evaporation resulting from the Hoffman degradation
and elimination of trimethylamine. Both compounds
were reported earlier by Beck et al. [2] and
Keene et al. [14] for MCM-41 templated by hexa-
decyltrimethylammonium chloride. At a relatively
low temperature 250–300°C fragmentation of the
alkyl chain takes also place producing shorter hydro-
carbons [15, 16].
Recently Kumar et al. [17] carried out
13
C CPMAS NMR studies of the thermal decomposi-
tion of the template CTAB at 200°C. They stated the
presence of N,N-dimethylhexadecylamine
CH
3
(CH
2
)
15
N(CH
3
)
2
as a product of CTAB decompo-
sition in MCM-41 surroundings.
In our previous paper [18] we demonstrated the
presence of 1-hexadecene and N,N-dimethylhexa-
decylamine in the liquid residue that condensed at the
outlet of the chromatographic column containing
MCM-41 sample heated up to 250°C in hydrogen
flow. Under these conditions we obtained MCM-41
silica synthesized by CTAB as a template possessing
emptied pores and structural parameters similar to
those of the calcined sample. Moreover, most of the
surface silanols were preserved, and their concentra-
tion was much higher than for the calcined sample.
In the present paper the results of similar experi-
ments for silica and silica–aluminium of the MCM-41
type are reported. The aim of this study was to give
some information on the chemical processes involved
in the surfactant removal in non-oxidizing atmosphere.
An additional aim of the present paper was to test how
aluminium incorporated into the framework of
MCM-41 mesoporous materials influences the re-
1388–6150/$20.00 Akadémiai Kiadó, Budapest, Hungary
© 2009 Akadémiai Kiadó, Budapest Springer, Dordrecht, The Netherlands
THERMAL DEGRADATION OF CTAB IN AS-SYNTHESIZED MCM-41
J. Goworek
1*
, Agnieszka Kierys
1
, W. Gac
2
, Anna Borówka
1
and R. Kusak
1
1
Department of Adsorption, Faculty of Chemistry, Maria Curie-Sk Óodowska University, Pl. M. Curie-SkÓodowskiej 3
20-031 Lublin, Poland
2
Department of Chemical Technology, Faculty of Chemistry, Maria Curie-Sk Óodowska University, Pl. M. Curie-SkÓodowskiej 3
20-031 Lublin, Poland
Thermal evacuation of a surfactant template from pure siliceous MCM-41 and MCM-41 containing aluminium in hydrogen flow
was investigated. Micelle templated MCM-41 were prepared using hexadecyltrimethylammonium bromide (CTAB). The products
of thermal surfactant degradation outside and inside pores were identified at various temperatures using
13
C solid-state nuclear mag-
netic resonance (NMR) spectroscopy, gas chromatography coupled with mass spectrometer (GC-MS) and temperature programmed
desorption coupled with mass spectrometer (TPD-MS). The GC-MS and
13
C MAS NMR results obtained from this study provide an
insight into the mechanism of surfactant transformation during MCM-41 synthesis on molecular level.
Keywords: CTAB, GC-MS, MAS NMR, MCM-41, template removal
* Author for correspondence: jgoworek@hermes.umcs.lublin.pl
Journal of Thermal Analysis and Calorimetry, Vol. 96 (2009) 2, 375–382