XANES characterization of extremely nanosized metal-carbonyl subspecies (Me = Cr, Mn, Fe, and Co) confined into the mesopores of MCM-41 materials

被引:45
作者
Ramallo-López, JM
Lede, EJ
Requejo, FG
Rodriguez, JA
Kim, JY
Rosas-Salas, R
Domínguez, JM
机构
[1] UNLP, FCE, Dto Fis, RA-1900 La Plata, Argentina
[2] Consejo Nacl Invest Cient & Tecn, IFLP, RA-1900 La Plata, Argentina
[3] Brookhaven Natl Lab, Dept Chem, Upton, NY 11973 USA
[4] Inst Mexicano Petr, Programa Ingn Mol, Mexico City 07730, DF, Mexico
关键词
D O I
10.1021/jp049241+
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A study of the stability, local order, and interaction of the surface silanol groups of MCM-41 with transition metal carbonyls M-x(CO)(y). (where M = Cr, Mn, Fe, Co) introduced by a chemical alternative method was performed by X-ray absorption near-edge spectroscopy (XANES). These molecular species, catalytically active for ethylene polymerization reactions, were previously characterized by FTIR and NMR in order to confirm their monodispersion and confined location into the mesopores of the MCM-41 material. Present experimental results indicate the high dispersion of metal species in all cases. Symmetry and stability depend on type of compound, Fe-carbonyl having the lowest stability. Changes in metal coordination and oxidation state are clearly followed by XANES indicating the interaction between sub-carbonyl species and the walls of the mesopores.
引用
收藏
页码:20005 / 20010
页数:6
相关论文
共 40 条
[21]   Pore-size control of cobalt dispersion and reducibility in mesoporous silicas [J].
Khodakov, AY ;
Griboval-Constant, A ;
Bechara, R ;
Villain, F .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (40) :9805-9811
[22]   ORDERED MESOPOROUS MOLECULAR-SIEVES SYNTHESIZED BY A LIQUID-CRYSTAL TEMPLATE MECHANISM [J].
KRESGE, CT ;
LEONOWICZ, ME ;
ROTH, WJ ;
VARTULI, JC ;
BECK, JS .
NATURE, 1992, 359 (6397) :710-712
[23]  
MANCEAU A, 1992, AM MINERAL, V77, P1133
[24]  
MANCEAU A, 1992, AM MINERAL, V77, P1144
[25]   Reversible coordination change of chromium in Cr-MCM-41 and Cr-MCM-48 studied by X-ray absorption near edge structure [J].
Pak, C ;
Haller, GL .
MICROPOROUS AND MESOPOROUS MATERIALS, 2001, 48 (1-3) :165-170
[26]   Manganese speciation in exhaust particulates of automobiles using MMT-containing gasoline [J].
Ressler, T ;
Wong, J ;
Roos, J .
JOURNAL OF SYNCHROTRON RADIATION, 1999, 6 :656-658
[27]   X-RAY ABSORPTION-SPECTROSCOPY OF IRON-TYROSINATE PROTEINS [J].
ROE, AL ;
SCHNEIDER, DJ ;
MAYER, RJ ;
PYRZ, JW ;
WIDOM, J ;
QUE, L .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1984, 106 (06) :1676-1681
[28]  
ROSASSALAS R, 2003, THESIS U NACIONAL AU
[29]  
Schulze Icking-Konert G., 1996, Phys. Rev. Lett, V76, P1047
[30]   EXAFS analyses of technetium(I) carbonyl complexes -: stability studies in solutions [J].
Seifert, S ;
Künstler, JU ;
Gupta, A ;
Funke, H ;
Reich, T ;
Hennig, C ;
Rossberg, A ;
Pietzsch, HJ ;
Alberto, R ;
Johannsen, B .
RADIOCHIMICA ACTA, 2000, 88 (3-4) :239-245