In situ generation of COx-free H2 by catalytic ammonia decomposition over Ru-Al-monoliths

Sabino Armenise; Fernando Cazaña; Antonio Monzón; Enrique García-Bordejé

doi:10.1016/j.fuel.2018.06.129

In situ generation of CO_x-free H₂ by catalytic ammonia decomposition over Ru-Al-monoliths

Sabino Armenise, Fernando Cazaña, Antonio Monzón, Enrique García-Bordejé

Research output: Contribution to journal › Article › peer-review

29 Scopus citations

Abstract

Ru catalysts supported on alumina coated monoliths has been prepared employing three different precursor, which are ruthenium chloride, ruthenium nitrosyl nitrate and ruthenium acetyl acetonate, by an equilibrium adsorption method. The Ru particle sizes could be controlled varying the metal precursor salt. Among the prepared catalysts, Ru catalyst prepared from nytrosyl nitrate exhibited the highest activity which is concomitant to the largest mean Ru particle size of 3.5 nm. The values of the apparent activation energy calculated from the Arrhenius equation are according to the Temkin-Phyzev model, indicating that the recombinative desorption of N ad-atoms is the rate-determining step of the reaction. However, the ratio between the kinetic orders with respect to ammonia and hydrogen (−α/β), is not in agreement to the valued predict by Temkin formalism. This fact could be related to the different operational conditions used during the reaction, and/or catalyst nature, but not to any change on the controlling step of the reaction.

Original language	English
Pages (from-to)	851-859
Number of pages	9
Journal	Fuel
Volume	233
DOIs	https://doi.org/10.1016/j.fuel.2018.06.129
State	Published - 1 Dec 2018

Bibliographical note

Funding Information:
The authors wants to acknowledge to the support of European Commission (FP7, Grant agreement n° 280658 ). Dr Armenise wants to acknowledge specially to University of Zaragoza , Instituto de Carboquímica and Banco Santander Hispano to finance the doctoral fellow. Finally the authors wants to acknowledge to Universida Politecnica Salesiana to provide the economical support to attend the IMCCRE-2018.

Funding Information:
The authors wants to acknowledge to the support of European Commission (FP7, Grant agreement n° 280658). Dr Armenise wants to acknowledge specially to University of Zaragoza, Instituto de Carboquímica and Banco Santander Hispano to finance the doctoral fellow. Finally the authors wants to acknowledge to Universida Politecnica Salesiana to provide the economical support to attend the IMCCRE-2018.

Publisher Copyright:
© 2018 Elsevier Ltd

Keywords

Ammonia decomposition
CO-free
Kinetics
Nanoparticle
Ru-catalyst
Structured reactors

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10.1016/j.fuel.2018.06.129

Cite this

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title = "In situ generation of COx-free H2 by catalytic ammonia decomposition over Ru-Al-monoliths",

abstract = "Ru catalysts supported on alumina coated monoliths has been prepared employing three different precursor, which are ruthenium chloride, ruthenium nitrosyl nitrate and ruthenium acetyl acetonate, by an equilibrium adsorption method. The Ru particle sizes could be controlled varying the metal precursor salt. Among the prepared catalysts, Ru catalyst prepared from nytrosyl nitrate exhibited the highest activity which is concomitant to the largest mean Ru particle size of 3.5 nm. The values of the apparent activation energy calculated from the Arrhenius equation are according to the Temkin-Phyzev model, indicating that the recombinative desorption of N ad-atoms is the rate-determining step of the reaction. However, the ratio between the kinetic orders with respect to ammonia and hydrogen (−α/β), is not in agreement to the valued predict by Temkin formalism. This fact could be related to the different operational conditions used during the reaction, and/or catalyst nature, but not to any change on the controlling step of the reaction.",

keywords = "Ammonia decomposition, CO-free, Kinetics, Nanoparticle, Ru-catalyst, Structured reactors",

author = "Sabino Armenise and Fernando Caza{\~n}a and Antonio Monz{\'o}n and Enrique Garc{\'i}a-Bordej{\'e}",

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doi = "10.1016/j.fuel.2018.06.129",

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AU - Armenise, Sabino

AU - Cazaña, Fernando

AU - Monzón, Antonio

AU - García-Bordejé, Enrique

PY - 2018/12/1

Y1 - 2018/12/1

N2 - Ru catalysts supported on alumina coated monoliths has been prepared employing three different precursor, which are ruthenium chloride, ruthenium nitrosyl nitrate and ruthenium acetyl acetonate, by an equilibrium adsorption method. The Ru particle sizes could be controlled varying the metal precursor salt. Among the prepared catalysts, Ru catalyst prepared from nytrosyl nitrate exhibited the highest activity which is concomitant to the largest mean Ru particle size of 3.5 nm. The values of the apparent activation energy calculated from the Arrhenius equation are according to the Temkin-Phyzev model, indicating that the recombinative desorption of N ad-atoms is the rate-determining step of the reaction. However, the ratio between the kinetic orders with respect to ammonia and hydrogen (−α/β), is not in agreement to the valued predict by Temkin formalism. This fact could be related to the different operational conditions used during the reaction, and/or catalyst nature, but not to any change on the controlling step of the reaction.

AB - Ru catalysts supported on alumina coated monoliths has been prepared employing three different precursor, which are ruthenium chloride, ruthenium nitrosyl nitrate and ruthenium acetyl acetonate, by an equilibrium adsorption method. The Ru particle sizes could be controlled varying the metal precursor salt. Among the prepared catalysts, Ru catalyst prepared from nytrosyl nitrate exhibited the highest activity which is concomitant to the largest mean Ru particle size of 3.5 nm. The values of the apparent activation energy calculated from the Arrhenius equation are according to the Temkin-Phyzev model, indicating that the recombinative desorption of N ad-atoms is the rate-determining step of the reaction. However, the ratio between the kinetic orders with respect to ammonia and hydrogen (−α/β), is not in agreement to the valued predict by Temkin formalism. This fact could be related to the different operational conditions used during the reaction, and/or catalyst nature, but not to any change on the controlling step of the reaction.

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