Atom-by-Atom Resolution of Structure–Function Relations over Low-Nuclearity Metal Catalysts
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Date
2019-06-24
Publication Type
Journal Article
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yes
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Abstract
Controlling the structure sensitivity of catalyzed reactions over metals is central to developing atom-efficient chemical processes. Approaching the minimum ensemble size, the properties enter a non-scalable regime in which each atom counts. Almost all trends in this ultra-small frontier derive from surface science approaches using model systems, because of both synthetic and analytical challenges. Exploiting the unique coordination chemistry of carbon nitride, we discriminate through experiments and simulations the interplay between the geometry, electronic structure, and reactivity of palladium atoms, dimers, and trimers. Catalytic tests evidence application-dependent requirements of the active ensemble. In the semi-hydrogenation of alkynes, the nuclearity primarily impacts activity, whereas the selectivity and stability are affected in Suzuki coupling. This powerful approach will provide practical insights into the design of heterogeneous catalysts comprising well-defined numbers of atoms.
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published
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Volume
58 (26)
Pages / Article No.
8724 - 8729
Publisher
Wiley-VCH
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Subject
C−C coupling; heterogeneous catalysis; hydrogenation; metal clusters; structure–activity relationships
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Funding
169679 - Doing more with less: efficient single-atom catalysts based on carbon nitride for sustainable chemical transformations (SNF)