ISSN 0012-5016, Doklady Physical Chemistry, 2012, Vol. 447, Part 1, pp. 210–212. © Pleiades Publishing, Ltd., 2012.
Original Russian Text © O.V. Surov, V.V. Vinogradov, N.Zh. Mamardashvili, O.I. Koifman, 2012, published in Doklady Akademii Nauk, 2012, Vol. 447, No. 3, pp. 304–307.
210
The search for materials with unique sorption
properties opens up new opportunities for the devel-
opment of prospective techniques for gas storage and
separation. Traditionally, physical adsorption of gases
is studied using materials with great specific surface
area and with developed porosity, such as activated
carbons, zeolites, and, lately, also carbon nanotubes
and porous organometallic structures. However,
organic molecular crystals are not usually considered
as potential adsorbents because they tend to form
close-packed nonporous structures [1]. Simple calix-
arene solvates are among the few examples that do not
obey this regularity.
Desolvation of calixarenes under controlled condi-
tions can be used to obtain a crystalline material with
active porous phase, which sorbs gases under standard
conditions [2, 3].
4-tert-Butylcalix[4]arene (t-BC) is a universal host
compound, which forms clathrates, or inclusion com-
pounds, with a variety of guests (solvents) [4, 5]. From
most of solvents, t-BC crystallizes to form tetragonal
1 : 1 or 1 : 2 host–guest complexes. Currently, two t-BC
polymorphs containing no solvent molecules in the
crystal lattice are known: α form obtained upon crys-
tallization from tetradecane (its structure consists of
close-packed dimers) in which the tert-butyl groups
are located in the cavities of the neighboring mole-
cules [6]; and β
0
form with a low packing coefficient
obtained by sublimation at 280°C under reduced pres-
sure [7] in which the t-BC molecules form the bilayer
packing motif with a slight shift. Heating of t-BC com-
plexes with solvents yields, depending on the desolva-
tion conditions, either the more dense self-associated
α form or low-density β
0
form [8].
Previously [9], we suggested that long-term
heat treatment of the t-BC complex with acetonitrile
(t-BC–AN) in vacuum at a temperature below 250°C
affords a partly solvated porous structure. This
assumption was verified by measuring low-tempera-
ture nitrogen adsorption on four t-BC samples, α and
β
0
forms, t-BC–AN complex, and partly desolvated
sample prepared by long-term heating in vacuum at
220°C. The N
2
adsorption and desorption isotherms
on the t-BC samples at 77 K are shown in Fig. 1.
For the α and β
0
forms and for the desolvated sam-
ple, the N
2
adsorption and desorption isotherms com-
pletely coincide (the desorption branches for α and β
forms are not shown in Fig. 1), whereas t-BC–AN
shows hysteresis over the whole range of relative pres-
sures. The isotherms for the α and β
0
forms are type II
isotherms according to the Brunauer classification [10],
while the isotherm for the partly desolvated sample
corresponds to type I, and the isotherm for the t-BC–
AN complex has distinctive features of both type I and
type II. The specific surface areas of the four t-BC
samples determined by the BET method are summa-
rized in the table.
PHYSICAL
CHEMISTRY
Microporous Structures
Based on 4-tert-Butylcalix[4]arene
O. V. Surov
a
, V. V. Vinogradov
a
, N. Zh. Mamardashvili
a
,
and Corresponding Member of the RAS O. I. Koifman
a, b
Received May 28, 2012
DOI: 10.1134/S0012501612110061
a
Krestov Institute of Solution Chemistry, Russian Academy
of Sciences, ul. Akademicheskaya 1, Ivanovo, 153045 Russia
b
Ivanovo State University of Chemical Technology,
pr. Engel’sa 7, Ivanovo, 153000 Russia
17.5
0 1.0
P/P
0
v, cm
3
/g (STP)
12.5
7.5
2.5
0.8 0.6 0.4 0.2
4
3
2
1
Fig. 1. Low-temperature nitrogen adsorption and desorp-
tion isotherms for t-BC samples: (1) α-form, (2) β
0
-form
(the desorption branches are not shown); (3) t-BC–AN
complex, (4) desolvated t-BC–AN complex (the adsorbed
N
2
volume is decreased fourfold in the plot). Dark symbols
correspond to sorption and light symbols, to desorption.