Effect of composition and pretreatment parameters on activity and stability of Cu-Al catalysts for water-gas shift reaction

Rasika B. Mane, Dae Woon Jeong, Atul V. Malawadkar, Hyunseog Roh, Chandrashekhar V. Rode

Research output: Contribution to journalArticle

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Abstract

We investigated various Cu species responsible for highly efficient Cu-Al oxide catalyst for the water-gas shift reaction (WGSR). The formation of various Cu species was achieved by systematically varying the Cu-Al composition in the coprecipitated mixed Cu-Al oxides. The Cu-Al composition of 70:30 (Cu-Al-7) was the best for WGSR using the reformate gas composition. In addition, the Cu-Al-7 catalyst reduced under 100 % H2, was relatively stable with time on stream of 100 h, at higher gas hourly space velocity of 36 201 h -1.The structural investigation of our coprecipitated catalysts with varying Cu-Al compositions revealed the formation of nonzero oxidation state copper and metallic Cu to be essential for the observed WGSR activity. In addition, the highest activity and stability of Cu-Al-7 catalysts reduced under 100 % H2 at lower temperature was attributed to particle-size stabilization and a lower extent of Cu aggregation by Cu2O and boehmite phases, respectively, along with the formation of various Cu species during the activation protocol for 12 h. Complete CO2 selectivity without methanation was observed for all the Cu-Al compositions irrespective of their pretreatment conditions. Teamwork brings success: The coexistence of various nonzero oxidation state and metallic copper species in a Cu-Al catalyst with 70 atom % Cu yields the highest CO conversion with a stable time on stream (TOS) of 100 h in the water-gas shift reaction (WGSR). PEM=proton-exchange membrane.

Original languageEnglish
Pages (from-to)1698-1706
Number of pages9
JournalChemCatChem
Volume6
Issue number6
DOIs
Publication statusPublished - 2014 Jan 1

Fingerprint

Water gas shift
pretreatment
catalysts
Catalysts
shift
Chemical analysis
gases
water
Oxides
Copper
methanation
Gases
copper
oxidation
oxides
Methanation
gas composition
Oxidation
Carbon Monoxide
stabilization

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Physical and Theoretical Chemistry
  • Organic Chemistry
  • Inorganic Chemistry

Cite this

Mane, Rasika B. ; Jeong, Dae Woon ; Malawadkar, Atul V. ; Roh, Hyunseog ; Rode, Chandrashekhar V. / Effect of composition and pretreatment parameters on activity and stability of Cu-Al catalysts for water-gas shift reaction. In: ChemCatChem. 2014 ; Vol. 6, No. 6. pp. 1698-1706.
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abstract = "We investigated various Cu species responsible for highly efficient Cu-Al oxide catalyst for the water-gas shift reaction (WGSR). The formation of various Cu species was achieved by systematically varying the Cu-Al composition in the coprecipitated mixed Cu-Al oxides. The Cu-Al composition of 70:30 (Cu-Al-7) was the best for WGSR using the reformate gas composition. In addition, the Cu-Al-7 catalyst reduced under 100 {\%} H2, was relatively stable with time on stream of 100 h, at higher gas hourly space velocity of 36 201 h -1.The structural investigation of our coprecipitated catalysts with varying Cu-Al compositions revealed the formation of nonzero oxidation state copper and metallic Cu to be essential for the observed WGSR activity. In addition, the highest activity and stability of Cu-Al-7 catalysts reduced under 100 {\%} H2 at lower temperature was attributed to particle-size stabilization and a lower extent of Cu aggregation by Cu2O and boehmite phases, respectively, along with the formation of various Cu species during the activation protocol for 12 h. Complete CO2 selectivity without methanation was observed for all the Cu-Al compositions irrespective of their pretreatment conditions. Teamwork brings success: The coexistence of various nonzero oxidation state and metallic copper species in a Cu-Al catalyst with 70 atom {\%} Cu yields the highest CO conversion with a stable time on stream (TOS) of 100 h in the water-gas shift reaction (WGSR). PEM=proton-exchange membrane.",
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Effect of composition and pretreatment parameters on activity and stability of Cu-Al catalysts for water-gas shift reaction. / Mane, Rasika B.; Jeong, Dae Woon; Malawadkar, Atul V.; Roh, Hyunseog; Rode, Chandrashekhar V.

In: ChemCatChem, Vol. 6, No. 6, 01.01.2014, p. 1698-1706.

Research output: Contribution to journalArticle

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T1 - Effect of composition and pretreatment parameters on activity and stability of Cu-Al catalysts for water-gas shift reaction

AU - Mane, Rasika B.

AU - Jeong, Dae Woon

AU - Malawadkar, Atul V.

AU - Roh, Hyunseog

AU - Rode, Chandrashekhar V.

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N2 - We investigated various Cu species responsible for highly efficient Cu-Al oxide catalyst for the water-gas shift reaction (WGSR). The formation of various Cu species was achieved by systematically varying the Cu-Al composition in the coprecipitated mixed Cu-Al oxides. The Cu-Al composition of 70:30 (Cu-Al-7) was the best for WGSR using the reformate gas composition. In addition, the Cu-Al-7 catalyst reduced under 100 % H2, was relatively stable with time on stream of 100 h, at higher gas hourly space velocity of 36 201 h -1.The structural investigation of our coprecipitated catalysts with varying Cu-Al compositions revealed the formation of nonzero oxidation state copper and metallic Cu to be essential for the observed WGSR activity. In addition, the highest activity and stability of Cu-Al-7 catalysts reduced under 100 % H2 at lower temperature was attributed to particle-size stabilization and a lower extent of Cu aggregation by Cu2O and boehmite phases, respectively, along with the formation of various Cu species during the activation protocol for 12 h. Complete CO2 selectivity without methanation was observed for all the Cu-Al compositions irrespective of their pretreatment conditions. Teamwork brings success: The coexistence of various nonzero oxidation state and metallic copper species in a Cu-Al catalyst with 70 atom % Cu yields the highest CO conversion with a stable time on stream (TOS) of 100 h in the water-gas shift reaction (WGSR). PEM=proton-exchange membrane.

AB - We investigated various Cu species responsible for highly efficient Cu-Al oxide catalyst for the water-gas shift reaction (WGSR). The formation of various Cu species was achieved by systematically varying the Cu-Al composition in the coprecipitated mixed Cu-Al oxides. The Cu-Al composition of 70:30 (Cu-Al-7) was the best for WGSR using the reformate gas composition. In addition, the Cu-Al-7 catalyst reduced under 100 % H2, was relatively stable with time on stream of 100 h, at higher gas hourly space velocity of 36 201 h -1.The structural investigation of our coprecipitated catalysts with varying Cu-Al compositions revealed the formation of nonzero oxidation state copper and metallic Cu to be essential for the observed WGSR activity. In addition, the highest activity and stability of Cu-Al-7 catalysts reduced under 100 % H2 at lower temperature was attributed to particle-size stabilization and a lower extent of Cu aggregation by Cu2O and boehmite phases, respectively, along with the formation of various Cu species during the activation protocol for 12 h. Complete CO2 selectivity without methanation was observed for all the Cu-Al compositions irrespective of their pretreatment conditions. Teamwork brings success: The coexistence of various nonzero oxidation state and metallic copper species in a Cu-Al catalyst with 70 atom % Cu yields the highest CO conversion with a stable time on stream (TOS) of 100 h in the water-gas shift reaction (WGSR). PEM=proton-exchange membrane.

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