Proton Conductivity versus Acidic Strength of One-Pot Synthesized Acid-Functionalized SBA-15 Mesoporous Silica

被引:16
作者
Bibent, Nicolas [1 ,2 ]
Mehdi, Ahmad [1 ]
Silly, Gilles [1 ]
Henn, Francois [1 ]
Devautour-Vinot, Sabine [1 ]
机构
[1] Univ Montpellier 2, Inst Charles Gerhardt Montpellier, UMR 5253, F-34095 Montpellier 5, France
[2] ICSM, UMR 5257, CNRS CEA ENSCM UM2, F-30207 Bagnols Sur Ceze, France
关键词
Self-assembly; Hybrid materials; Organic-inorganic hybrid composites; Mesoporous materials; Conducting materials; SULFONIC-ACID; PHOSPHONIC ACID; PROTOGENIC GROUP; POROUS SILICA; WATER; PORE; NMR; MCM-41; ADSORPTION; RELAXATION;
D O I
10.1002/ejic.201100186
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
This paper reports on the one-pot synthesis and characterization of the functionalized mesoporous SBA-15 silica, which contains two loadings of the different acid groups [CO2H, PO(OH)(2) and SO3H]. The thermodynamic features of the water that was confined in these porous silicas was investigated by Differential Scanning Calorimetry (DSC). The results showed that the melting behaviour of the confined water was mainly governed by the pore diameter and, as a consequence, indicated that the chemical "decoration" of the porous surface did not play a key role in the water thermodynamics. On the contrary, the proton conductivity of the hydrated mesoporous materials, which was examined under a wide range of temperatures (-100 to 70 degrees C), was strongly dependent on both the physical state of the confined water and the acidity of the functional groups that were located at the porous surface. The proton conductivity was shown to be directly related to the pK(a) and the density of the functional groups attached to the mesopore surface. The high conductivity values that were obtained at a low temperature when the confined water is frozen, led us to postulate that the SO3H-functionalized SBA-15 sample could be a promising candidate for electrolyte solid applications in fuel cells.
引用
收藏
页码:3214 / 3225
页数:12
相关论文
共 76 条
[1]   Tetrahedral displacement: The molecular mechanism behind the Debye relaxation in water (vol 100, pg 1073, 1996) [J].
Agmon, N .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (21) :4352-4352
[2]   Direct synthesis of ordered mesoporous silica containing iodopropyl groups.: A useful function for chemical modifications [J].
Alauzun, Johan ;
Mehdi, Ahmad ;
Reye, Catherine ;
Corriu, Robert .
NEW JOURNAL OF CHEMISTRY, 2007, 31 (06) :911-915
[3]   Direct synthesis of bifunctional mesoporous organosilicas containing chelating groups in the framework and reactive functional groups in the channel pores [J].
Alauzun, Johan ;
Mehdi, Ahmad ;
Reye, Catherine ;
Corriu, Robert J. P. .
JOURNAL OF MATERIALS CHEMISTRY, 2007, 17 (04) :349-356
[4]   Porous silica and polysilsesquioxane with covalently linked phosphonates and phosphonic acids [J].
Aliev, A ;
Ou, DL ;
Ormsby, B ;
Sullivan, AC .
JOURNAL OF MATERIALS CHEMISTRY, 2000, 10 (12) :2758-2764
[5]   Broadband dielectric spectroscopy of water confined in MCM-41 molecular sieve materials -: low-temperature freezing phenomena [J].
Banys, J ;
Kinka, M ;
Macutkevic, J ;
Völkel, G ;
Böhlmann, W ;
Umamaheswari, V ;
Hartmann, M ;
Pöppl, A .
JOURNAL OF PHYSICS-CONDENSED MATTER, 2005, 17 (19) :2843-2857
[6]   THE DETERMINATION OF PORE VOLUME AND AREA DISTRIBUTIONS IN POROUS SUBSTANCES .1. COMPUTATIONS FROM NITROGEN ISOTHERMS [J].
BARRETT, EP ;
JOYNER, LG ;
HALENDA, PP .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1951, 73 (01) :373-380
[7]   A NEW FAMILY OF MESOPOROUS MOLECULAR-SIEVES PREPARED WITH LIQUID-CRYSTAL TEMPLATES [J].
BECK, JS ;
VARTULI, JC ;
ROTH, WJ ;
LEONOWICZ, ME ;
KRESGE, CT ;
SCHMITT, KD ;
CHU, CTW ;
OLSON, DH ;
SHEPPARD, EW ;
MCCULLEN, SB ;
HIGGINS, JB ;
SCHLENKER, JL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (27) :10834-10843
[8]   HETERONUCLEAR DECOUPLING IN ROTATING SOLIDS [J].
BENNETT, AE ;
RIENSTRA, CM ;
AUGER, M ;
LAKSHMI, KV ;
GRIFFIN, RG .
JOURNAL OF CHEMICAL PHYSICS, 1995, 103 (16) :6951-6958
[9]  
Brovchenko I., 2008, INTERFACIAL CONFINED
[10]   NEW METHOD FOR SIMULTANEOUS DETERMINATION OF SIZE AND SHAPE OF PORES - THERMOPOROMETRY [J].
BRUN, M ;
LALLEMAND, A ;
QUINSON, JF ;
EYRAUD, C .
THERMOCHIMICA ACTA, 1977, 21 (01) :59-88