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Linker driven site-specific catalysis in atomically precise silver cluster assemblies.

Priyanka Chandrashekar1, Arun Karmakar2, Ravari Kandy Aparna1

  • 1School of Chemistry, Indian Institute of Science Education and Research Thiruvananthapuram Kerala 69551 India sukhendu@iisertvm.ac.in.

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|March 6, 2025
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Summary
This summary is machine-generated.

Atomically precise silver (Ag12) nanoclusters with varying linkers demonstrate tunable catalytic activity for the hydrogen evolution reaction (HER). The Ag12-pyrazine assembly shows superior performance due to synergistic effects between the cluster and linker.

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Area of Science:

  • Materials Science
  • Catalysis
  • Electrochemistry

Background:

  • Metal nanoclusters (NCs) offer atomic-level insights into catalytic mechanisms.
  • Constructing integrated catalysts with molecular understanding, especially for silver (Ag) clusters, remains challenging.

Purpose of the Study:

  • To demonstrate atomically precise Ag12 cluster assemblies as paradigms for the hydrogen evolution reaction (HER).
  • To investigate how cluster core and linker functional units fine-tune catalytic activity.
  • To elucidate the mechanism of site-specific catalysis in these assemblies.

Main Methods:

  • Synthesis and characterization of Ag12 cluster assemblies with pyridine, pyrazine, bipyridine, bis(pyridyl)ethane, and azopyridine linkers.
  • Electrochemical studies to evaluate hydrogen evolution reaction (HER) activity.
  • Theoretical calculations and structural analysis to understand reaction mechanisms.

Main Results:

  • Ag12 cluster assemblies exhibit tunable HER catalytic activity based on the linker.
  • The Ag12-pyrazine (Ag12-pyz) assembly shows significantly enhanced catalytic activity and selective hydrogen adsorption.
  • Synergy between the Ag12 cluster and the pyrazine linker drives site-specific catalysis.

Conclusions:

  • This work provides a structural model for understanding catalyst active sites and activity in functional cluster-based assemblies.
  • The findings advance the development of efficient and selective catalysts for HER.
  • Ag12-pyz serves as a highly efficient catalyst due to its unique linker properties and inter-cluster interactions.