Splitting of Hydrogen Atoms into Proton-Electron Pairs at BaO-Ru Interfaces for Promoting Ammonia Synthesis under Mild Conditions

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Ru catalysts promoted with alkali and alkaline earthhave shownsuperior ammonia (NH3) synthesis activities under mildconditions. Although these promoters play a vital role in enhancingcatalytic activity, their function has not been clearly understood.Here, we synthesize a series of Ba-Ru/MgO catalysts with an optimalRu particle size (similar to 2.3 nm) and tailored BaO-Ru interfacialstructures. We discover that the promoting effect is created throughthe separate storage of H+/e(-) pairs atthe BaO-Ru interface. Chemisorbed H atoms on Ru dissociateinto H+/e(-) pairs at the BaO-Ruinterface, where strongly basic, nonreducible BaO selectively capturesH(+) while leaving e(-) on Ru. The resultingelectron accumulation in Ru facilitates N-2 activation viaenhanced pi-backdonation and inhibits hydrogen poisoning duringNH(3) synthesis. Consequently, the formation of intimateBaO-Ru interface without an excessive loss of accessible Rusites enables the synthesis of highly active catalysts for NH3 synthesis.
Publisher
AMER CHEMICAL SOC
Issue Date
2023-05
Language
English
Article Type
Article
Citation

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.145, no.20, pp.11364 - 11374

ISSN
0002-7863
DOI
10.1021/jacs.3c02529
URI
http://hdl.handle.net/10203/310484
Appears in Collection
CH-Journal Papers(저널논문)CBE-Journal Papers(저널논문)
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