Mechanistic insights into interfacial nano-synergistic effects in trimetallic Rh-on-NiCo on-CNTs for room temperature solvent-free hydrogenations

Mono- and bimetallic nanoparticles (NPs) supported on carbon nanotubes (CNTs) (Ni/CNTs, Co/CNTs and NiCo/CNTs) were synthesized at room temperature (RT) via hydrazine hydrate reduction method without any surfactant. The galvanic replacement reaction was exploited to prepare Rh/Ni/CNTs, Rh/Co/CNTs and Rh/NiCo/CNTs supported nanocatalysts. Prepared nanocatalysts were extensively characterized using an array of advanced analytical techniques. The catalytic performance of the catalysts was evaluated in the hydrogenation of tetralin. Reduced Rh/NiCo/CNTs catalyst (Rh-on-NiCo NP) exhibited high catalytic activity at RT, significantly improved as compared to Rh/Ni/CNTs and Rh/Co/CNTs due to the interfacial nano-synergy effect among different metallic related species (Rh, Ni and Co). In-situ XAS results confirmed the mechanism of the interfacial nano-synergy effect, wherein Rh sites provided activated hydrogen species (H*), and H* was subsequently transferred to the surface of NiCo NPs; while tetralin was adsorbed and activated at NiCo sites, reacting with H* to produce decalin. The present work proposed a novel strategy to design highly efficient and stable multimetallic catalysts for heterogeneous catalytic hydrogenation reactions. © 2021

Authors
Zhu L.1 , Zhu H.2 , Shakouri M.5 , Zeng L.1 , Yang Z.2 , Hu Y.5 , Ye H.2 , Wang H. 6 , Chen B.H.3 , Luque R. 4, 7
Publisher
Elsevier B.V.
Language
English
Status
Published
Number
120404
Volume
297
Year
2021
Organizations
  • 1 College of Chemistry and Chemical Engineering, Faculty of Materials Metallurgy and Chemistry, Jiangxi University of Science and Technology, Ganzhou, Jiang Xi 341000, China
  • 2 Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, China
  • 3 Department of Chemical and Biochemical Engineering, National Engineering Laboratory for Green Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China
  • 4 Departamento de Química Orgánica, Universidad de Córdoba, Campus de Rabanales, Edificio Marie Curie (C-3), Ctra Nnal IV, Km 396, Córdoba, E14071, Spain
  • 5 Canadian Light Source, Inc., University of Saskatchewan, 44 Innovation Boulevard, Saskatoon, SK S7N 2V3, Canada
  • 6 Department of Chemical and Biological Engineering, University of Saskatchewan, Saskatoon, SK S7N 5A9, Canada
  • 7 Peoples Friendship University of Russia (RUDN University), 6 Miklukho Maklaya str., Moscow, 117198, Russian Federation
Keywords
Carbon nanotubes; Hydrogenation reaction; Interfacial nano-synergy effect; Room temperature; Trimetallic catalyst
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