Abstract
The development of alternative methods to the Haber-Bosch process for ammonia (NH(3)) synthesis is a pressing and formidable challenge. Nuclear energy represents a low-carbon, efficient and stable source of power. The harnessing of nuclear energy to drive nitrogen (N(2)) reduction not only allows 'green' NH(3) synthesis, but also offers the potential for the storage of nuclear energy as a readily transportable zero-carbon fuel. Herein, we explore radiocatalytic N(2) fixation to NH(3) induced by γ-ray radiation. Hydrated electrons (e(-) (aq)) that are generated from water radiolysis enable N(2) reduction to produce NH(3). Ru-based catalysts synthesized by using γ-ray radiation with excellent radiation stability substantially improve NH(3) production in which the B(5) sites of Ru particles may play an important role in the activation of N(2). By benefitting from the remarkable penetrating power of γ-ray radiation, radiocatalytic NH(3) synthesis can proceed in an autoclave under appropriate pressure conditions, resulting in an NH(3) concentration of ≤5.1 mM. The energy conversion efficiency of the reaction is as high as 563.7 mg(NH3)·MJ(-1). This radiocatalytic chemistry broadens the research scope of catalytic N(2) fixation while offering promising opportunities for converting nuclear energy into chemical energy.