New Ammonia Synthesis Catalysts Based on Supported Potassium Carbonyl Ruthenates as Precursors of Catalytically Active Ruthenium Particles and Potassium Promoter

New Ammonia Synthesis Catalysts Based on Supported Potassium Carbonyl Ruthenates as Precursors of Catalytically Active Ruthenium Particles and Potassium Promoter Научная публикация

Журнал

Journal of Molecular Catalysis A: Chemical
ISSN: 1381-1169

Вых. Данные

Год: 2004, Том: 219, Номер: 1, Страницы: 149-153 Страниц : 5 DOI: 10.1016/j.molcata.2004.04.031

Авторы

Yunusov S.M. ¹ , Kalyuzhnaya E.S. ¹ , Moroz B.L. ² , Ivanova A.S. ² , Reshetenko T.V. ² , Avdeeva L.B. ² , Likholobov V.A. ² , Shur V.B. ¹

Организации

1	A.N. Nesmeyanov Institute of Organoelement Compounds, Russian Academy of Sciences, Vavilov Street 28, Moscow 119991, Russia
2	K.G. Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Ac. Lavrent’ev Avenue 5, Novosibirsk 630090, Russia

New supported “single-component” ruthenium catalysts for ammonia synthesis are reported. For preparation of the catalysts, various potassium carbonyl ruthenates such as K2[Ru6(CO)18] (K:Ru=1:3), K4[Ru4(CO)12] (K:Ru=1:1), K6[Ru6(CO)16] (K:Ru=1:1), K6[Ru4(CO)11] (K:Ru=1.5:1) and K2[Ru(CO)4] (K:Ru=2:1) were used as precursors of both catalytically active ruthenium particles and potassium promoter while graphite-like carbon “Sibunit” was utilized as a support. The studied catalysts have been compared in their activity with the previously described K2[Ru4(CO)13]-based catalyst (K:Ru=1:2) on “Sibunit”. It has been established that the rate of the ammonia synthesis at 300 °C over these catalysts increases with the increase in the K:Ru ratio in the starting carbonyl metallate, reaching a maximum in the case of the K6[Ru4(CO)11]-based sample. On further enhancement in the K:Ru ratio, i.e. when the K2[Ru(CO)4] catalyst is used, the rate of the ammonia formation noticeably diminishes. The activity of the K2[Ru(CO)4]-based catalyst in the ammonia synthesis can be considerably augmented on the replacement of “Sibunit” by catalytic filamentous carbon CFC-III or MgO. The use of γ-Al2O3 or carbon-coated γ-Al2O3 as supports decreases the reaction rate. An introduction of metallic potassium into the K2[Ru(CO)4] catalysts on “Sibunit” and CFC-III accelerates strongly the process of the ammonia synthesis. The highest activity is exhibited by the K2[Ru(CO)4]+K system on “Sibunit” at the metallic potassium to carbon molar ratio of 0.08. On using this catalyst (3.55 g), the steady ammonia concentration in the gas flow at 300 °C and 1 atm amounts to 71.1% of the equilibrium value while at 350 and 400 °C the process of the ammonia synthesis fully reaches the equilibrium. In its efficiency in the ammonia production at 250–300 °C, the K2[Ru(CO)4]+K catalyst on “Sibunit” carbon significantly exceeds the previously developed K2[Ru4(CO)13]+K catalyst on the same support.

Yunusov S.M. , Kalyuzhnaya E.S. , Moroz B.L. , Ivanova A.S. , Reshetenko T.V. , Avdeeva L.B. , Likholobov V.A. , Shur V.B.
New Ammonia Synthesis Catalysts Based on Supported Potassium Carbonyl Ruthenates as Precursors of Catalytically Active Ruthenium Particles and Potassium Promoter
Journal of Molecular Catalysis A: Chemical. 2004. V.219. N1. P.149-153. DOI: 10.1016/j.molcata.2004.04.031 WOS Scopus РИНЦ CAPlusCA OpenAlex Sciact

Поступила в редакцию:	21 янв. 2004 г.
Принята к публикации:	30 апр. 2004 г.
Опубликована online:	7 июн. 2004 г.
Опубликована в печати:	1 сент. 2004 г.

Web of science:	WOS:000222878700018
Scopus:	2-s2.0-3042793151
РИНЦ:	13455835
Chemical Abstracts:	2004:561886
Chemical Abstracts (print):	142:267420
OpenAlex:	W2047001997
Sciact:	9912

БД	Цитирований
Scopus	14
OpenAlex	14