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Ligand effects in catalysis by atomically precise gold nanoclusters.

Xian-Kai Wan1,2, Jia-Qi Wang1, Zi-Ang Nan1,2

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Protecting ligands on gold nanoclusters significantly impact their catalytic activity. Alkynyl-protected gold nanoclusters show high activity in alkyne semihydrogenation, unlike thiolated versions.

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Area of Science:

  • Heterogeneous catalysis
  • Nanomaterials science
  • Surface chemistry

Background:

  • Atomically precise gold nanoclusters serve as model catalysts due to their defined structures.
  • Investigating ligand effects requires isolating ligand type as the sole variable.
  • Controlling ligand spheres is crucial for tuning nanocluster catalytic performance.

Purpose of the Study:

  • To synthesize and compare two isostructural gold nanoclusters with different protecting ligands.
  • To evaluate the catalytic performance of these nanoclusters in alkyne semihydrogenation.
  • To elucidate the role of protecting ligands in hydrogen activation and catalytic efficiency.

Main Methods:

  • Direct reduction synthesis of isostructural Au38 nanoclusters: [Au38(L)20(Ph3P)4]2+ where L is alkynyl or thiolate.
  • Characterization of nanocluster structure, including an unprecedented fcc-type Au34 kernel.
  • Testing catalytic activity of supported nanoclusters (on TiO2) in the semihydrogenation of alkynes.

Main Results:

  • Alkynyl-protected Au38 nanoclusters exhibited high activity (>97%) in alkyne semihydrogenation.
  • Thiolated Au38 nanoclusters showed very low conversion (<2%) in the same reaction.
  • The significant difference in activity highlights the critical role of protecting ligands in H2 activation.

Conclusions:

  • Protecting ligands are a key factor in modulating the catalytic performance of gold nanoclusters.
  • The choice of ligand sphere can drastically alter catalytic efficiency, particularly in reactions involving H2 activation.
  • This study demonstrates precise control over ligand construction to tune gold nanocluster catalysis.