Ammonia synthesis over lanthanoid oxide-supported ruthenium catalysts

被引：36
作者：
Miyahara, Shin-ichiro [1 ]
Sato, Katsutoshi [1 ,2 ]
Kawano, Yukiko [3 ]
Imamura, Kazuya [3 ,4 ]
Ogura, Yuta [1 ]
Tsujimaru, Kotoko [3 ]
Nagaoka, Katsutoshi [1 ]
机构：
[1] Nagoya Univ, Grad Sch Engn, Dept Chem Syst Engn, Chikusa Ku, Furo Cho, Nagoya, Aichi 4648603, Japan
[2] Kyoto Univ, Elements Strategy Initiat Catalysts & Batteries E, Nishikyo Ku, 1-30 Goryo Ohara, Kyoto 6158245, Japan
[3] Oita Univ, Fac Sci & Technol, Dept Integrated Sci & Technol, 700 Dannoharu, Oita 8701192, Japan
[4] Kochi Univ, Fac Sci & Technol, Dept Chem & Biotechnol, Res Lab Hydrothermal Chem, 2-5-1 Akebono Cho, Kochi 7808520, Japan
来源：
CATALYSIS TODAY | 2021年 / 376卷 / 376期
关键词：
Renewable energy; Energy carrier; Kinetic study; Hydrogen poisoning; Ruthenium catalyst; LOW-CRYSTALLINE; RU CATALYST; HYDROGEN; EFFICIENT; KINETICS;
D O I：
10.1016/j.cattod.2020.08.031
中图分类号：
O69 [应用化学];
学科分类号：
081704 ;
摘要：
Ammonia synthesis catalysts with high activity under mild reaction conditions for use in synthetic chemical processes powered by renewable energy are needed. Here, we investigated the physicochemical properties and ammonia synthesis activity of lanthanoid oxide-supported Ru catalysts. The basicity of the Ru/lanthanoid oxide catalysts, as estimated by CO2 temperature-programmed desorption, was higher than that of Ru/MgO, a representative catalyst with high ammonia synthesis activity, and a positive relationship was observed between basicity and turnover frequency. The turnover frequency of Ru/Pr2O3 and Ru/La2O3 (both 0.24 s(-1)) was eight times that of Ru/MgO (0.03 s(-1)). A kinetic analysis revealed that hydrogen poisoning, which is a typical drawback of oxide-supported Ru catalysts, was markedly retarded in the Ru/lanthanoid oxide catalysts. As a result, the ammonia synthesis rate of the Ru/Pr2O3 catalyst increased with increasing reaction pressure, reaching 49 mmol g(-1) h(-1) at 400 degrees C and 1.0 MPa, which was 12 times that of Ru/MgO under the same conditions.
引用
收藏
页码：36 / 40
页数：5
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