Abstract
It is of great significance for upgrading single-atom catalysts (SACs) to further improve their intrinsic catalytic activities while maintaining the merits of maximum atom utilization and high selectivity. Here, we report a simple and practical strategy to construct phosphorus (P) atom bridged ruthenium (Ru) ensemble (Ru-P-Ru) in carbon skeleton, which is achieved by redispersing Ru clusters with C-P species and in-situ generated PH3. The turnover frequency of the Ru-P-Ru catalyst is 9-fold higher than that of the RuP4 SAC in the selective hydrodeoxygenation of o-phthalic anhydride, as well as other diverse hydrogenations of C=X bonds (X = O, C, N) with good recyclability. Experimental and computational studies reveal that the d-band centers of Ru in the Ru-P-Ru are closer to the Fermi level than that of isolated Ru SAC, significantly promoting the absorption and activation of substrates. This fabrication strategy is also applicable to other M-P-M catalysts, enriching the knowledge of atomically dispersed catalysts.
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