Solid-state nuclear magnetic resonance study of acetone oxime adsorbed on CuZSM-5 and on HZSM-5

Wu, J; Larsen, S C

doi:10.1006/jcat.1998.2340

Title: Solid-state nuclear magnetic resonance study of acetone oxime adsorbed on CuZSM-5 and on HZSM-5

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Abstract

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 intactmore »« less

Authors:

Wu, J; Larsen, S C ^[1]

Univ. of Iowa, Iowa City, IA (United States). Dept. of Chemistry

Publication Date:: Mon Feb 15 00:00:00 EST 1999

OSTI Identifier:: 328303

Resource Type:: Journal Article

Journal Name:: Journal of Catalysis

Additional Journal Information:: Journal Volume: 182; Journal Issue: 1; Other Information: PBD: 15 Feb 1999

Country of Publication:: United States

Language:: English

Subject:: 54 ENVIRONMENTAL SCIENCES; OXIMES; ADSORPTION; ZEOLITES; SORPTIVE PROPERTIES; REACTION INTERMEDIATES; NITRIC OXIDE; SELECTIVE CATALYTIC REDUCTION; PROPANE; CHEMICAL REACTION KINETICS

Citation Formats


                    Wu, J, and Larsen, S C. Solid-state nuclear magnetic resonance study of acetone oxime adsorbed on CuZSM-5 and on HZSM-5.  United States: N. p., 1999. 
        Web.  doi:10.1006/jcat.1998.2340.

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                    Wu, J, & Larsen, S C. Solid-state nuclear magnetic resonance study of acetone oxime adsorbed on CuZSM-5 and on HZSM-5.  United States.  https://doi.org/10.1006/jcat.1998.2340

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                    Wu, J, and Larsen, S C. 1999.  
        "Solid-state nuclear magnetic resonance study of acetone oxime adsorbed on CuZSM-5 and on HZSM-5".  United States.  https://doi.org/10.1006/jcat.1998.2340.

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@article{osti_328303,

  title        = {Solid-state nuclear magnetic resonance study of acetone oxime adsorbed on CuZSM-5 and on HZSM-5},

  author       = {Wu, J and Larsen, S C},

  abstractNote = {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.},

  doi          = {10.1006/jcat.1998.2340},

  url          = {https://www.osti.gov/biblio/328303},
  journal      = {Journal of Catalysis},
number       = 1,

  volume       = 182,

  place        = {United States},

  year         = {Mon Feb 15 00:00:00 EST 1999},

  month        = {Mon Feb 15 00:00:00 EST 1999}

}

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