Atmospheric-pressure ammonia synthesis on AuRu catalysts enabled by plasmon-controlled hydrogenation and nitrogen-species desorption
/ Authors
L. Yuan, Briley B. Bourgeois, Elijah Begin, Yirui Zhang, Alan X. Dai, Zhihua Cheng, Amy S. McKeown-Green, Zhichen Xue, Yi Cui, Kun Xu
and 6 more authors
Y. Wang, Matthew R. Jones, Yi Cui, Arun Majumdar, Junwei Lucas Bao, J. Dionne
/ Abstract
The Haber–Bosch process for ammonia synthesis contributes up to ~3% of global greenhouse gas emissions. Plasmonic catalysts strongly concentrate light and can alter the reaction intermediates via out-of-equilibrium processes, providing the potential for an alternative, less-energy-intensive pathway to synthesize ammonia. Here we show that gold-ruthenium (AuRu) bimetallic nanoparticles can synthesize ammonia at room temperature and pressure using visible light. We create AuRu alloys with varying compositions and achieve ammonia production rates of ~60 μmol per gram of catalyst bed per hour. In situ infrared spectroscopy reveals that light accelerates the hydrogenation of nitrogen intermediates compared to conventional thermal catalysis. Through computational modelling, we demonstrate that photo-excited electrons enable associative hydrogenation pathways for nitrogen activation rather than direct nitrogen–nitrogen bond breaking. This light-assisted mechanism requires both hydrogen and light working together to overcome the nitrogen activation barrier, mimicking how biological enzymes produce ammonia naturally and providing fundamental insights for developing sustainable, energy-efficient chemical synthesis. Conventional ammonia synthesis is energy intensive. Here the authors explore the mechanism of light-driven ammonia synthesis through in situ spectroscopy and modelling, and demonstrate that certain AuRu plasmonic alloys are promising catalysts for this potentially more sustainable process.
Journal: Nature Energy