Makepeace Joshua W, Wood Thomas J, Hunter Hazel M A, Jones Martin O, David William I F
ISIS Facility , Rutherford Appleton Laboratory , Harwell Oxford , Didcot , OX11 0QX , UK . Email:
Inorganic Chemistry Laboratory , University of Oxford , Oxford , OX1 3QR , UK.
Chem Sci. 2015 Jul 1;6(7):3805-3815. doi: 10.1039/c5sc00205b. Epub 2015 May 7.
We demonstrate that non-stoichiometric lithium imide is a highly active catalyst for the production of high-purity hydrogen from ammonia, with superior ammonia decomposition activity to a number of other catalyst materials. Neutron powder diffraction measurements reveal that the catalyst deviates from pure imide stoichiometry under ammonia flow, with active catalytic behaviour observed across a range of stoichiometry values near the imide. These measurements also show that hydrogen from the ammonia is exchanged with, and incorporated into, the bulk catalyst material, in a significant departure from existing ammonia decomposition catalysts. The efficacy of the lithium imide-amide system not only represents a more promising catalyst system, but also broadens the range of candidates for amide-based ammonia decomposition to include those that form imides.
我们证明,非化学计量比的锂亚胺是一种用于从氨生产高纯度氢气的高活性催化剂,其氨分解活性优于许多其他催化剂材料。中子粉末衍射测量表明,在氨气流下,该催化剂偏离了纯亚胺化学计量比,在亚胺附近的一系列化学计量比值范围内观察到了活性催化行为。这些测量还表明,氨中的氢与块状催化剂材料发生交换并掺入其中,这与现有的氨分解催化剂有很大不同。锂亚胺 - 酰胺体系的有效性不仅代表了一种更有前景的催化剂体系,还拓宽了基于酰胺的氨分解候选材料的范围,使其包括那些形成亚胺的材料。