A transient kinetic investigation of Ni-catalyzed methanation: Annual report

Godbole, G G; Goodwin, Jr, J G

Title: A transient kinetic investigation of Ni-catalyzed methanation: Annual report

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Abstract

The most important objective of this research is to gain an insight into the nature of the main surface species involved during methanation and to develop an understanding of factors influencing the rate determining process. With this ultimate goal in mind, studies of the reaction pathways of oxygen (and oxygen containing surface species) have been conducted. From experiments carried out by adding water to the gas phase and switching between isotopes H/sub 2//sup 16/O, H/sub 2//sup 18/O and D/sub 2//sup 16/O, it was concluded that oxygen, once reacted to form water, does not apparently readsorb. However, hydrogen in the water molecule can be readily exchanged with hydrogen on the surface, perhaps by an Eley-Rideal type of mechanism. By following multiple transients of carbon and oxygen, simultaneously, during /sup 12/CO-/sup 13/CO switch experiments, it was found that the residence time (and hence the size of the precursor adsorbed species reservoir) of water is either equal to or greater than that of methane, depending upon the reaction conditions and the catalyst employed. Future experiments planned include transients by switching between /sup 16/O/sub 2/ and /sup 18/O/sub 2/ under reaction conditions. These experiments, along with those already carried out, will be able tomore »« less

Authors:: Godbole, G G; Goodwin, Jr, J G

Publication Date:: Fri May 01 00:00:00 EDT 1987

Research Org.:: Pittsburgh Univ., PA (USA). Dept. of Chemical and Petroleum Engineering

OSTI Identifier:: 6307843

Report Number(s):: DOE/ER/13624-1
ON: DE87013944

DOE Contract Number:: FG02-86ER13624

Resource Type:: Technical Report

Resource Relation:: Other Information: Portions of this document are illegible in microfiche products

Country of Publication:: United States

Language:: English

Subject:: 10 SYNTHETIC FUELS; METHANATION; CATALYSIS; CARBON 13; CATALYSTS; DEUTERIUM; NICKEL; OXYGEN; OXYGEN 18; REACTION INTERMEDIATES; RESEARCH PROGRAMS; WATER; CARBON ISOTOPES; CHEMICAL REACTIONS; ELEMENTS; EVEN-EVEN NUCLEI; EVEN-ODD NUCLEI; HYDROGEN COMPOUNDS; HYDROGEN ISOTOPES; ISOTOPES; LIGHT NUCLEI; METALS; NONMETALS; NUCLEI; ODD-ODD NUCLEI; OXYGEN COMPOUNDS; OXYGEN ISOTOPES; STABLE ISOTOPES; TRANSITION ELEMENTS; 090121* - Hydrocarbon Fuels- Chemical Synthesis- (1976-1989)

Citation Formats


                    Godbole, G G, and Goodwin, Jr, J G. A transient kinetic investigation of Ni-catalyzed methanation: Annual report.  United States: N. p., 1987. 
        Web.

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                    Godbole, G G, & Goodwin, Jr, J G. A transient kinetic investigation of Ni-catalyzed methanation: Annual report.  United States.

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                    Godbole, G G, and Goodwin, Jr, J G. 1987.  
        "A transient kinetic investigation of Ni-catalyzed methanation: Annual report".  United States.

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@article{osti_6307843,

  title        = {A transient kinetic investigation of Ni-catalyzed methanation: Annual report},

  author       = {Godbole, G G and Goodwin, Jr, J G},

  abstractNote = {The most important objective of this research is to gain an insight into the nature of the main surface species involved during methanation and to develop an understanding of factors influencing the rate determining process. With this ultimate goal in mind, studies of the reaction pathways of oxygen (and oxygen containing surface species) have been conducted. From experiments carried out by adding water to the gas phase and switching between isotopes H/sub 2//sup 16/O, H/sub 2//sup 18/O and D/sub 2//sup 16/O, it was concluded that oxygen, once reacted to form water, does not apparently readsorb. However, hydrogen in the water molecule can be readily exchanged with hydrogen on the surface, perhaps by an Eley-Rideal type of mechanism. By following multiple transients of carbon and oxygen, simultaneously, during /sup 12/CO-/sup 13/CO switch experiments, it was found that the residence time (and hence the size of the precursor adsorbed species reservoir) of water is either equal to or greater than that of methane, depending upon the reaction conditions and the catalyst employed. Future experiments planned include transients by switching between /sup 16/O/sub 2/ and /sup 18/O/sub 2/ under reaction conditions. These experiments, along with those already carried out, will be able to focus on the long-debated issue in the literature about whether or not the most abundant reaction intermediate (MARI) during methanation is an oxygen containing species. Future experiments will also include studies on a series of Ni and Ru catalysts in order to understand the effect of initial carbon deposition on methanation.},

  doi          = {},

  url          = {https://www.osti.gov/biblio/6307843},
  journal      = {},
number       = ,

  volume       = ,

  place        = {United States},

  year         = {Fri May 01 00:00:00 EDT 1987},

  month        = {Fri May 01 00:00:00 EDT 1987}

}

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