Ammonia decomposition over La-doped Al2O3 supported Co catalyst

Abstract

As the hydrogen source of carbon-free fuel cells, the key to realize the green and low-energy decomposition hydrogen production process is to select materials with excellent catalytic performance for ammonia dehydrogenation. In this study, the rare earth element lanthanum (La) was doped onto the surface of Al2O3 by the impregnation method. The aforementioned material was subsequently used as a new material for the synthesis of single metal Co catalysts that catalyzed ammonia decomposition. Various characterization techniques (XRD, HRTEM, N2 physical adsorption-desorption, ICP, XPS, SEM, H2-TPR) were employed to investigate the relationship between the structure and performance of Co/La–Al2O3 catalysts. The findings indicated that the 10Co/La(5)-Al2O3 catalyst was the most active. Under the conditions of 550 °C and 9000 mL h−1·gcat−1, the conversion of ammonia reached 90 %, and the yield of hydrogen reached 8.9 mmol·gcat−1·min−1. A perovskite-type metal oxide layer of LaAlO3 was generated on the surface of Al2O3 support after doping the appropriate amount of lanthanum (5 %), which directly affects the catalytic performance of the catalyst. The small amount of LaAlO3 optimized the strong interaction between the metal Co and the supports, thereby enhancing catalytic performance. While stabilizing the active component Co, XPS and H2-TPR also implied that the presence of La could enhance the electron transfer between the support and Co, as well as facilitate the desorption of nitrogen and hydrogen products, therefore, the low temperature activity of Co/La–Al2O3 catalyst can be improved. The ammonia decomposition efficiency of the catalyst doped with 5 % wt La was much higher than that of the catalyst without La incorporation. The simple modified support developed by us, which loads a monoatomic Co catalyst, provides a new approach for the development of high-activity transition metal catalysts.