Mu Bo-Shuai, Xu Yang, Tu Zhiyu, Zhang Yugang, Liang Weiqiu, Li Jiahao, Wang Xianglin, Shen Siyong, Chen Junyi, Liu Zhibo
Beijing National Laboratory for Molecular Sciences, Radiochemistry and Radiation Chemistry Key Laboratory of Fundamental Science, Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of Education, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, China.
Peking University-Tsinghua University Center for Life Sciences, Peking University, Beijing 100871, China.
Natl Sci Rev. 2024 Aug 30;11(11):nwae302. doi: 10.1093/nsr/nwae302. eCollection 2024 Nov.
The development of alternative methods to the Haber-Bosch process for ammonia (NH) 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) reduction not only allows 'green' NH synthesis, but also offers the potential for the storage of nuclear energy as a readily transportable zero-carbon fuel. Herein, we explore radiocatalytic N fixation to NH induced by γ-ray radiation. Hydrated electrons (e ) that are generated from water radiolysis enable N reduction to produce NH. Ru-based catalysts synthesized by using γ-ray radiation with excellent radiation stability substantially improve NH production in which the B sites of Ru particles may play an important role in the activation of N. By benefitting from the remarkable penetrating power of γ-ray radiation, radiocatalytic NH synthesis can proceed in an autoclave under appropriate pressure conditions, resulting in an NH concentration of ≤5.1 mM. The energy conversion efficiency of the reaction is as high as 563.7 mg·MJ. This radiocatalytic chemistry broadens the research scope of catalytic N fixation while offering promising opportunities for converting nuclear energy into chemical energy.
开发替代哈伯-博施法的氨(NH₃)合成方法是一项紧迫且艰巨的挑战。核能是一种低碳、高效且稳定的能源。利用核能驱动氮(N₂)还原不仅可以实现“绿色”氨合成,还为将核能储存为易于运输的零碳燃料提供了潜力。在此,我们探索γ射线辐射诱导的放射性催化氮固定为氨的过程。水辐射分解产生的水合电子(e⁻)能够使氮还原生成氨。通过γ射线辐射合成的具有优异辐射稳定性的钌基催化剂可显著提高氨的产量,其中钌颗粒的B位可能在氮的活化中起重要作用。得益于γ射线辐射卓越的穿透能力,放射性催化氨合成可在高压釜中于适当压力条件下进行,氨浓度可达≤5.1 mM。该反应的能量转换效率高达563.7 mg·MJ⁻¹。这种放射性催化化学拓宽了催化氮固定的研究范围,同时为将核能转化为化学能提供了有前景的机会。