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Alkenes undergo reduction by the addition of molecular hydrogen to give alkanes. Because the process generally occurs in the presence of a transition-metal catalyst, the reaction is called catalytic hydrogenation.
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Catalytic hydrogenation of alkenes is a transition-metal catalyzed reduction of the double bond using molecular hydrogen to give alkanes. The mode of hydrogen addition follows syn stereochemistry.
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The Synthesis, Characterization and Reactivity of a Series of Ruthenium N-triphosPh Complexes
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Correlating Single-Atomic Ruthenium Interdistance with Long-Range Interaction Boosts Hydrogen Evolution Reaction

Bowen Jiang1,2, Jiawei Zhu1, Zhenzhi Xia1

  • 1State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, P. R. China.

Advanced Materials (Deerfield Beach, Fla.)
|November 15, 2023
PubMed
Summary

Researchers developed correlated single-atom catalysts (c-SACs) with precisely controlled metal-metal distances. Optimizing the single-atomic distance (SAD) significantly enhanced catalytic activity, offering a new method for catalyst design.

Keywords:
HERlong-range interactionmolecular designrutheniumsingle-atom catalystssingle-atomic interdistance

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Area of Science:

  • Materials Science
  • Catalysis
  • Nanotechnology

Background:

  • Correlated single-atom catalysts (c-SACs) show enhanced performance over conventional catalysts due to tailored intersite metal-metal interactions.
  • Precise quantification of single-atomic distance (SAD) is crucial for understanding and improving c-SAC catalytic kinetics but remains challenging.

Purpose of the Study:

  • To develop a method for fabricating c-SACs with precisely controlled SAD.
  • To investigate the relationship between SAD and catalytic activity in ruthenium (Ru) c-SACs.
  • To provide insights into the catalytic mechanisms governed by metal-site interactions.

Main Methods:

  • Fabrication of three Ru c-SACs using a planar organometallic molecular design and π-π molecule-carbon nanotube confinement.
  • Graded SAD achieved, ranging from 2.4 to 9.3 Å.
  • Density functional theory (DFT) calculations to analyze electronic structure and catalytic activity.

Main Results:

  • Tailoring Ru SAD to 7.0 Å resulted in exceptional turnover frequency (17.92 H₂ s⁻¹) and mass activity (100.4 A mg⁻¹).
  • Achieved performance surpasses previously reported Ru-based catalysts.
  • DFT calculations confirmed a negative correlation between Ru SAD and its d-band center, optimizing catalytic activity.

Conclusions:

  • The developed method enables experimental quantification of metal SAD in c-SACs.
  • Optimized SAD is critical for maximizing catalytic efficiency in c-SACs.
  • This work offers valuable insights into the catalytic mechanisms of c-SACs and a pathway for designing superior catalysts.