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Dispersed surface Ru ensembles on MgO(111) for catalytic ammonia decomposition

Huihuang Fang, Simson Wu, Tugce Ayvali, Jianwei Zheng, Joshua Fellowes, Ping-Luen Ho, Kwan Chee Leung, Alexander Large, Georg Held, Ryuichi Kato, Kazu Suenaga, Yves Ira A. Reyes, Ho Viet Thang, Hsin-Yi Tiffany Chen and Shik Chi Edman Tsang ()
Additional contact information
Huihuang Fang: University of Oxford
Simson Wu: University of Oxford
Tugce Ayvali: University of Oxford
Jianwei Zheng: University of Oxford
Joshua Fellowes: University of Oxford
Ping-Luen Ho: University of Oxford
Kwan Chee Leung: University of Oxford
Alexander Large: Diamond Light Source
Georg Held: Diamond Light Source
Ryuichi Kato: National Institute of Advanced Industrial Science and Technology (AIST)
Kazu Suenaga: National Institute of Advanced Industrial Science and Technology (AIST)
Yves Ira A. Reyes: National Tsing Hua University
Ho Viet Thang: University of Science and Technology
Hsin-Yi Tiffany Chen: National Tsing Hua University
Shik Chi Edman Tsang: University of Oxford

Nature Communications, 2023, vol. 14, issue 1, 1-15

Abstract: Abstract Ammonia is regarded as an energy vector for hydrogen storage, transport and utilization, which links to usage of renewable energies. However, efficient catalysts for ammonia decomposition and their underlying mechanism yet remain obscure. Here we report that atomically-dispersed Ru atoms on MgO support on its polar (111) facets {denoted as MgO(111)} show the highest rate of ammonia decomposition, as far as we are aware, than all catalysts reported in literature due to the strong metal-support interaction and efficient surface coupling reaction. We have carefully investigated the loading effect of Ru from atomic form to cluster/nanoparticle on MgO(111). Progressive increase of surface Ru concentration, correlated with increase in specific activity per metal site, clearly indicates synergistic metal sites in close proximity, akin to those bimetallic N2 complexes in solution are required for the stepwise dehydrogenation of ammonia to N2/H2, as also supported by DFT modelling. Whereas, beyond surface doping, the specific activity drops substantially upon the formation of Ru cluster/nanoparticle, which challenges the classical view of allegorically higher activity of coordinated Ru atoms in cluster form (B5 sites) than isolated sites.

Date: 2023
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DOI: 10.1038/s41467-023-36339-w

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