4.8 Article

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

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 145, 期 20, 页码 11364-11374

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.3c02529

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Ba-Ru/MgO catalysts are synthesized with an optimal Ru particle size and tailored BaO-Ru interfacial structures, which create a promoting effect through the separate storage of H+/e(-) pairs at the BaO-Ru interface. Chemisorbed H atoms on Ru dissociate into H+/e(-) pairs at the BaO-Ru interface, where selective capture of H(+) by strongly basic, nonreducible BaO leaves e(-) on Ru. The resulting electron accumulation in Ru facilitates N-2 activation and inhibits hydrogen poisoning during NH(3) synthesis.
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.

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