Interface engineering is a significance strategy to afford efficient selective oxidation for supported catalysts. Herein, constructing of frustrated Lewis pairs (FLPs) sites on CeO 2 and supporting Au-Pd nanoparticles to provide a highly selective production of 2,5-furandicarboxylic acid (FDCA) from 2,5-bis(hydroxymethyl)furan (BHMF). Mechanism investigations illustrate that the FLPs active sites enhance the adsorption and activation of catalyst for BHMF, decreasing the activation energy of rate-determining step. Simultaneously, the FLPs sites induce the electron transfer of the catalyst, generating a novel Au-Pd-CeO 2 interface that promotes the adsorption of molecule oxygen and the formation of the superoxide radical. Thereby, the Au x Pd y /P T -CeO 2 catalysts enable superior catalytic performance, achieving a satisfactory turnover frequency of 55.29 h −1 and a highly FDCA yield of 94.0 %. Such interfacial FLPs sites exhibit the great potentials for the selective oxidation of various unsaturated compounds.
DePing Chen,ZhenYi Shao,LiRong Yang,Ying Chen,Yanghong Wei,Zhihua Hu,Liyang Cai,Yifan Zhang,Xun He
The design of efficient electrocatalysts for ethanol oxidation is essential for commercializing direct ethanol fuel cells (DEFCs). In this strategy, a mesoporous carbon microsphere (MC) was first synthesized by inverting the micro-emulsion technique. The MC@Au/Pd catalyst with a particular core-shell structure was obtained by utilizing mesoporous carbon as a core to load the Au/Pd layer. The novelty of the MC@Au/Pd catalyst with specialized core-shell structures lies not only in the high specific surface area inherited from the carbon core but also in the strong electronic interactions caused by the lattice mismatch between the core (Au) and shell (Pd) atoms. Particularly, electrochemical measures demonstrated that the Au/Pd catalyst exhibits superior catalytic activity toward the ethanol oxidation reaction (EOR) compared with commercial Pd/C catalysts. This is mainly due to the high specific surface area and mesoporous pore size inherited from the core carbon microspheres. In addition, the mesoporous carbon core and Au/Pd shell in the well-organized core-shell catalyst (MC@Au/Pd) influence the catalytic activity for ethanol oxidation by adjusting the electronic structure of Pd.
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