Chinese Journal of Catalysis ›› 2012, Vol. 33 ›› Issue (7): 1191-1197.DOI: 10.3724/SP.J.1088.2012.20233

• Research papers • Previous Articles     Next Articles

Effect of Hydrothermal Treatment of Activated Carbon by Nitric Acid on Activity of Ba-Ru-K/AC Catalyst for Ammonia Synthesis

FENG Guoquan, LAN Guojun, LI Ying, HAN Wenfeng, LIU Huazhang*   

  1. Institute of Industrial Catalysis, Zhejiang University of Technology, Hangzhou 310032, Zhejiang, China
  • Received:2012-02-16 Revised:2012-03-22 Online:2012-06-21 Published:2012-06-21

Abstract: Activated carbon (AC) was functionalized by HNO3 hydrothermal treatment at 180 oC. Ruthenium catalyst samples were prepared through incipient wetness impregnation with aqueous solution of RuCl3·3H2O precursor. The influence of HNO3 concentration on the support structure, surface oxygen functional groups (SOFGs), Ru dispersion, and the catalytic activity of Ru/AC for ammonia synthesis was investigated by N2 physisorption, He temperature-programmed desorption, CO chemisorption, and transmission electron microscopy. The results indicated that the amount of SOFGs, Ru particle size, and activity depend strongly on the HNO3 concentration used in the hydrothermal treatment. The porous texture of carbon support almost keeps unchanged with low HNO3 concentrations (≤ 2.0 mol/L) treatment, while it decreases significantly at high acid concentrations (2.4 mol/L). However, the amount of SOFGs increases with the concentration of nitric acid as well as the Ru particle size. Ammonia synthesis activity of the Ba-Ru-K/AC catalyst samples, whose support was treated with HNO3 (2.0 mol/L), is as high as 17.80% at 400 oC, 10 MPa, and 10000 h−1, which is 16.8% higher than that of the catalyst obtained via washing with HNO3 (4.6 mol/L). The optimal conditions of hydrothermal treatment are HNO3 (2.0 mol/L) at 150 oC for 4 h with filling degree 70%. Therefore, the amount of SOFGs and Ru particle size are tunable by varying the HNO3 concentration during the hydrothermal treatment.

Key words: activated carbon, hydrothermal treatment, surface oxygen functional group, barium, ruthenium, potassium, dispersion, ammonia synthesis