Ru Single Atom and Nanoparticle Tandem Catalyst Unlocking High-Efficiency Ammonia Synthesis under Mild Conditions

作者：Yanliang Zhou, Bo Yang, Lu Wang, Kailin Su, Ben Liu, Hongpeng Fang, Kexin Yue, Xiuyun Wang, Haifeng Qi, Lirong Zheng, Wei Li, Lilong Jiang · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c09736 · 被引用次数：30 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Catalytic Processes in Materials Science、Nanomaterials for catalytic reactions

The development of highly efficient catalysts that enable Haber–Bosch ammonia (NH 3 ) synthesis under mild conditions remains critically challenging since the competitive activation of coadsorbates, particularly excessive N 2 or H 2 binding at active sites, is a trade-off and detrimental to NH 3 synthesis. Herein, we design a novel Ru tandem catalyst that combines Ru single atom (Ru 1 ) with nanoparticle sites (Ru NP ) on CeO 2 nanoislands, leveraging cascade hydrogen catalysis between functionally distinct Ru sites to realize highly efficient NH 3 synthesis under mild conditions. Our studies reveal that Ru NP sites suffer from hydrogen poisoning, whereas Ru 1 sites exclusively adsorb N 2 . The hydrogen spillover from Ru NP to Ru 1 sites reduces hydrogen coverage on Ru NP sites to effectively decrease the N 2 dissociation barrier and also greatly facilitates N 2 hydrogenation at Ru 1 sites for NH 3 synthesis, thus overcoming the trade-off in the dynamic N 2 /H 2 activation equilibrium. As a result, the Ru single atom and nanoparticle tandem catalyst achieves a remarkable NH 3 synthesis rate of 59.0 mmol g cat –1 h –1 with 600 h long-term operational stability at 400 °C and 1 MPa, possessing an exceptionally high specific rate among reported Ru-based catalysts. This catalyst structure design paves a new path for NH 3 synthesis under mild conditions.