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Nature of =~SiOCrO(2)CI And (=~SiO)(2)CrO(2) Sites Prepared By Grafting CrO(2)CI(2) Onto Silica

Journal Article · · J. Phys. Chem. C112:6439,2008
OSTI ID:958585
The room-temperature reaction between chromyl chloride and Sylopol 952 silicas pretreated at 200, 450, and 800 C was investigated using IR, XANES, and EXAFS spectroscopy, as well as by DFT modeling. On the silicas pretreated at 200 and 450 C, the structurally uniform sites formed by the reaction with one surface hydroxyl group are described as {triple_bond}SiOCrO{sub 2}Cl. Unreacted silanols persist on these silicas even in the presence of excess CrO{sub 2}Cl{sub 2}, and on the silica pretreated at 200 C some participate in hydrogen bonding with the grafted monochlorochromate sites. On the silica pretreated at 800 C, both {triple_bond}SiOCrO{sub 2}Cl and ({triple_bond}SiO){sub 2}CrO{sub 2} sites are formed. The latter are produced despite the absence of hydrogen-bonded hydroxyl pairs on the support. The origin of the chromate sites is proposed to be the reaction between CrO{sub 2}Cl{sub 2} and hydroxyl-substituted siloxane 2-rings. These rings are likely formed at 800 C by condensation between a pair of vicinal silanols in which one of the silanols is also a member of a geminal pair.
Research Organization:
Stanford Linear Accelerator Center (SLAC)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC02-76SF00515
OSTI ID:
958585
Report Number(s):
SLAC-REPRINT-2009-108
Journal Information:
J. Phys. Chem. C112:6439,2008, Journal Name: J. Phys. Chem. C112:6439,2008 Journal Issue: 16 Vol. 112; ISSN 1932-7447
Country of Publication:
United States
Language:
English