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Noble-metal free catalysts for ammonia dehydrogenation within permeation membrane reactors for improved conversion
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DOI：10.1039/D5GC06003F.png)
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Abstract
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Ammonia is a carbon-free hydrogen carrier that can be easily transported; but ammonia decomposition catalysts have historically relied on ruthenium. However; less scarce nickel-based catalysts have difficulties in performing ammonia decomposition as efficiently as ruthenium-based catalysts; as nickel-based catalysts are passivated by the hydrogen produced during the reaction. One way to circumvent this issue is to utilize a permeation membrane reactor that removes the hydrogen product during reaction. Here; we report the ammonia decomposition activity of less costly nickel-based trimetallic catalysts at temperature ranges that are compatible with permeation membrane reactors. A variety of nickel-based catalysts were synthesized to test the effect of the alkali (Na; K; Rb; and Cs) and alkaline earth metal (Ca; Sr; and Ba) promoter on the ammonia decomposition efficiency. The performance of the catalyst was highly dependent on the alkali or alkaline earth metal promoter utilized; with Rb demonstrating the strongest promotion. The best performing catalyst; 12%Ni/4%Yb/12%Rb/Al2O3 was tested in a permeation membrane reactor and achieved >99.9% ammonia conversion at >30 cm3 NH3 gcat−1 min−1. Additionally; the 12%Ni/4%Yb/12%Rb/Al2O3 catalysts maintained >90% of its initial activity after exposure to air for six months without reactivation.
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