Ammonia synthesis over ruthenium supported on modified zirconia: Relationships between the catalyst structure and activity

WANG Zi-qing; LIN Jian-xin; WANG Rong; WEI Ke-mei

Volume 40 Issue 12

Dec. 2012

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WANG Zi-qing, LIN Jian-xin, WANG Rong, WEI Ke-mei. Ammonia synthesis over ruthenium supported on modified zirconia: Relationships between the catalyst structure and activity[J]. Journal of Fuel Chemistry and Technology, 2012, 40(12): 1472-1479.

Citation:

WANG Zi-qing, LIN Jian-xin, WANG Rong, WEI Ke-mei. Ammonia synthesis over ruthenium supported on modified zirconia: Relationships between the catalyst structure and activity[J]. Journal of Fuel Chemistry and Technology, 2012, 40(12): 1472-1479.

Citation:

WANG Zi-qing, LIN Jian-xin, WANG Rong, WEI Ke-mei. Ammonia synthesis over ruthenium supported on modified zirconia: Relationships between the catalyst structure and activity[J]. Journal of Fuel Chemistry and Technology, 2012, 40(12): 1472-1479.

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Ammonia synthesis over ruthenium supported on modified zirconia: Relationships between the catalyst structure and activity

National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, China

Received Date: 2012-05-17
Rev Recd Date: 2012-07-14
Publish Date: 2012-12-31

Abstract

Abstract

Modified zirconia (ZrO₂) were synthesized by high temperature calcination of ZrO(OH)₂ gels digested in alkalic solution; with the modified ZrO₂ as support, ruthenium catalysts for ammonia synthesis were prepared with K₂RuO₄ solution. The catalysts were characterized by X-ray diffraction (XRD), temperature programmed reduction of hydrogen (H₂-TPR), temperature programmed desorption of CO₂ (CO₂-TPD), nitrogen sorption, X-ray fluorescence spectroscopy (XRF), and CO chemisorption; the relationship between the catalyst structure and its catalytic activity was especially discussed. The results revealed that the digestion either in KOH or NH₄OH solution can enhance the surface area of the ZrO₂ support, while digestion in KOH is able to obtain the support with high basicity, which benefits to getting the ruthenium catalyst of high activity. The strong basicity of the modified ZrO₂ support, rather than the high ruthenium dispersion, plays a more important role in enhancing the activity of the supported ruthenium catalyst. For ammonia synthesis under 425 ℃, 5 MPa and a space velocity of 10 000 h^-1, NH₃ outlet concentration over Ru/ZrO₂-KOH is 5.96%, which is 11%, 143% and 103% higher than those of K-Ru/ZrO₂-NH₄OH, K-Ru/ZrO₂-CP and Ru/ZrO₂-NH₄OH, respectively.
- digestion in basic solution,
- zircona,
- ruthenium,
- ammonia synthesis,
- basicity

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References(34)

References

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