First-principles calculations of ammonia decomposition on Ni(110) surface

► The barrier of the associative desorption of N is higher than those of NHx (x = 1-3) dehydrogenation. ► At 350 K, the associative desorption of N is the rate determining step. ► Ni(110) is more active for NH3 decomposition than Ni(111) and Ni(211). ► NH3 decomposition over Ni-based catalysts shows a remarkable structure-sensitivity.