Uniphase ruthenium-iridium alloy-based electronic regulation for electronic structure-function study in methane oxidation to methanol

For the first time, we synthesize uniphase face-centered-cubic (fcc) structured Ru-Ir alloy nanoparticles (NPs) with a uniform size of ∼2 nm over the whole composition range, using RuCl3 and IrCl4 as precursors. The electronic structure of Ir is gradually tuned by varying the composition. The consistency of the fcc structure of Ru and Ir within the RuxIr1-x alloys allows better study of the electronic structure-activity relationship without introducing unnecessary factors such as the lattice/phase effect in the case of the RuIr alloy composed of different structures of hcp-Ru and fcc-Ir. The obtained RuxIr1-x alloys were further employed as precursors for the synthesis of their corresponding oxides, RuxIr1-xO2/CuO, to probe the electronic structure-activity relationship in the methane oxidation to methanol reaction. The electronic structure of Ir4+ was able to be regulated by tuning the composition of the RuxIr1-x NP precursors. The optimum catalytic behavior was achieved over Ru0.5Ir0.5O2/CuO, where both Ru and Ir reached the highest electrophilic state, at which point the C-H cleavage capacity also reached the maximum as observed by CH4-TPR. © 2020 The Royal Society of Chemistry.

Yang L. 1 , Huang J. 1 , Dai S.2 , Tang X.2 , Hu Z.1 , Li M.3 , Zeng H.1 , Luque R. 4, 5 , Duan P.6 , Rui Z.1
Royal Society of Chemistry
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  • 1 School of Chemical Engineering and Technology, Guangdong Engineering Technology Research Center for Platform Chemicals from Marine Biomass and Their Functionalization, Sun Yat-sen University, Zhuhai, 519082, China
  • 2 Key Laboratory for Advanced Materials, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, China
  • 3 Polymer Program, Institute of Materials Science, University of Connecticut, Storrs, CT 06269, United States
  • 4 Departamento de Química Orgánica, Universidad de Córdoba, Campus de Rabanales Edificio Marie Curie (C-3), Ctra Nnal IV-A, Km 396, Cordoba, E14014, Spain
  • 5 Peoples Friendship University of Russia (RUDN University), 6 Miklukho-Maklaya Str., Moscow, 117198, Russian Federation
  • 6 Shaanxi Key Laboratory of Energy Chemical Process Intensification, School of Chemical Engineering and Technology, Xi'an Jiaotong University, No. 28, West Xianning Road, Xi'an, Shaanxi, 710049, China
Ключевые слова
Binary alloys; Chlorine compounds; Electronic structure; Methane; Methanol; Ruthenium alloys; Structures (built objects); Synthesis (chemical); Alloy nanoparticle; Catalytic behavior; Composition ranges; Different structure; Face-centered cubic; Methane oxidation; Structure activity relationships; Structure-function studies; Iridium alloys
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