The construction of bimetallic sites with strong interaction can effectively regulate the electronic structure and modulate the adsorption behavior of adsorbate species on bimetallic catalysts,thereby overcoming catal...The construction of bimetallic sites with strong interaction can effectively regulate the electronic structure and modulate the adsorption behavior of adsorbate species on bimetallic catalysts,thereby overcoming catalytic bottlenecks.Herein,an RhPb bimetallene(RhPb b-ML)with the strong d-p orbital hybridization is proposed for efficiently catalyzing ethanol oxidation reaction(EOR).Notably,the specific EOR activity of RhPb b-ML is 32 and 6.8 times higher than those of Rh metallene and commercial Pt/C,respectively.Theoretical calculation analysis reveals that the introduction of Pb atoms into the Rh lattice leads to an upward shift of the d-band center of Rh on RhPb(111).The shift in the d-band center is primarily attributed to the different degrees of hybridization between the d sub-orbitals of Rh and the p-orbitals of Pb,which enhance the adsorption of key species and improve EOR activity and selectivity.In-situ infrared tests and high-performance liquid chromatography tests together confirm that RhPb b-ML not only exhibits enhanced ability for the breakage of C-C bonds but also effectively suppresses the generation of absorbed CO.Furthermore,the strategy of enhancing catalyst performance through the strong d-p orbital hybridization has been demonstrated to be scalable to other bimetallic catalysts,providing valuable insights for the design of advanced catalysts.展开更多
基金supported by the National Natural Science Foundation of China(22309108,22202076,22272103)the China Postdoctoral Science Foundation(2022M711231,2023TQ0204)+3 种基金the Science and Technology Innovation Team of Shaanxi Province(2023-CX-TD27)the Fundamental Research Funds for the Central Universities(GK202202001)the 111 Project(B14041)Sanqin scholars'innovation teams in Shaanxi Province,China。
文摘The construction of bimetallic sites with strong interaction can effectively regulate the electronic structure and modulate the adsorption behavior of adsorbate species on bimetallic catalysts,thereby overcoming catalytic bottlenecks.Herein,an RhPb bimetallene(RhPb b-ML)with the strong d-p orbital hybridization is proposed for efficiently catalyzing ethanol oxidation reaction(EOR).Notably,the specific EOR activity of RhPb b-ML is 32 and 6.8 times higher than those of Rh metallene and commercial Pt/C,respectively.Theoretical calculation analysis reveals that the introduction of Pb atoms into the Rh lattice leads to an upward shift of the d-band center of Rh on RhPb(111).The shift in the d-band center is primarily attributed to the different degrees of hybridization between the d sub-orbitals of Rh and the p-orbitals of Pb,which enhance the adsorption of key species and improve EOR activity and selectivity.In-situ infrared tests and high-performance liquid chromatography tests together confirm that RhPb b-ML not only exhibits enhanced ability for the breakage of C-C bonds but also effectively suppresses the generation of absorbed CO.Furthermore,the strategy of enhancing catalyst performance through the strong d-p orbital hybridization has been demonstrated to be scalable to other bimetallic catalysts,providing valuable insights for the design of advanced catalysts.
