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Unveiling Long-Range Wavelike Alternately Competitive and Cooperative Bond Coupling Modes in Single-Atom Catalysis
Jun Zhou1, Jiani Jiang1, Yangyang Li2
1Institute of Industry Chemistry, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China.
Abstract:
Supports can critically influence or even dominate the chemical state, adsorption property, and catalytic performance of single-atom catalysts (SACs), but the fundamental physicochemical principles driving adsorbate-M1-ligand-support bond interactions have not been fully understood yet. Here, we reveal the orbital-level interaction modes underlying the long-range bond couplings in SACs by using single-atom Ru (Ru1) supported on rutile-type oxides (TiO2, SnO2, and MnO2) in CO adsorption and oxidation as a model system. Our results show that Ru1-support binding strength and catalytic activity for CO oxidation increase in the following order: Ru1/TiO2 < Ru1/SnO2 < Ru1/MnO2, while CO-Ru1 adsorption strength oppositely decreases as Ru1/TiO2 > Ru1/SnO2 > Ru1/MnO2. These interaction trends are overall controlled by the reactivity of surface lattice oxygen atoms (Osl) on supports. We further discover an alternating competitive and cooperative bond coupling mode in the heteroatomic chains of adsorbate-M1-ligand-support systems, in which the strengths of adjacent bonds competitively suppress, while alternating bonds cooperatively enhance. This wavelike bond coupling mode provides a new point to understand support effects on SAC-support interactions and structure-function relationships in SACs.
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