Solid-state nuclear magnetic resonance study of acetone oxime adsorbed on CuZSM-5 and on HZSM-5
- Univ. of Iowa, Iowa City, IA (United States). Dept. of Chemistry
The reactions of acetone oxime, a proposed reaction intermediate for the selective catalytic reduction (SCR) of NO with propane on CuZSM-5 and on HZSM-5, have been studied with {sup 13}C and {sup 15}N solid-state magic-angle spinning nuclear magnetic resonance (MAS NMR). The carbon- and/or nitrogen-containing surface species, as well as the products formed under conditions of thermodynamic equilibrium, have been monitored and identified. In the absence of NO and after heating to 150--200 C, the main hydrolysis products of adsorbed acetone oxime on CuZSM-5 are acetone and hydroxylamine, while the main hydrolysis products on HZSM-5 are acetic acid and methylamine. In addition, N{sub 2} and N{sub 2}O are formed from acetone oxime adsorbed on both HZSM-5 and CuZSM-5. In the presence of {sup 15}NO, the observation of mixed-labeled {sup 14}N{sup 15}NO and {sup 15N}{sup 14}NO shows that new N-N bonds are formed over CuZSM-5 and HZSM-5 between two different nitrogen atoms: one from gaseous {sup 15}NO molecules and the other from adsorbed acetone oxime and/or acetone oxime hydrolysis products. When {sup 15}NO and unlabeled acetone oxime are reacted on CuZSM-5, the {sup 14}N{sup 15}NO/{sup 15}N{sup 14}NO ratio is approximately 3, suggesting that the NO bond of gas-phase NO remains intact when it reacts with acetone oxime to form N{sub 2}O. It is also found that the formation of new N-N bonds from the reaction of NO and acetone oxime occurs at room temperature on CuZSM-5, but not until {approximately}150 C on HZSM-5.
- OSTI ID:
- 328303
- Journal Information:
- Journal of Catalysis, Vol. 182, Issue 1; Other Information: PBD: 15 Feb 1999
- Country of Publication:
- United States
- Language:
- English
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