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Atomically Precise Au24Pt(thiolate)12(dithiolate)3 Nanoclusters with Excellent Electrocatalytic Hydrogen Evolution
Miyu Sera1, Sakiat Hossain2, Sara Yoshikawa1
1Department of Applied Chemistry, Faculty of Science, Tokyo University of Science, Kagurazaka, Shinjuku-ku, Tokyo 162-8601, Japan.
Journal of the American Chemical Society
|October 15, 2024
Summary
New gold-platinum (Au-Pt) alloy nanoclusters show significantly enhanced activity for the hydrogen evolution reaction (HER). These precisely structured catalysts offer superior performance compared to existing platinum nanoparticle catalysts.
Area of Science:
- Nanomaterials Science
- Catalysis
- Electrochemistry
Background:
- Gold-platinum (Au-Pt) alloy nanoclusters are emerging as promising catalysts for the hydrogen evolution reaction (HER).
- Previous studies demonstrated the high activity of [Au24Pt(C6)18]0 for HER, highlighting the potential of well-defined nanostructures.
Purpose of the Study:
- To synthesize and characterize novel Au-Pt alloy nanoclusters with tailored ligand shells.
- To investigate the structure-activity relationship of these new nanoclusters in electrocatalytic HER.
Main Methods:
- Ligand exchange reactions on a precursor Au-Pt nanocluster ([Au24Pt(PET)18]0).
- Synthesis of new clusters using mono- and dithiolate ligands, including 4-tert-butylbenzenethiolate (TBBT), thiodithiolate (TDT), and 1,3-propanedithiolate (PDT).
- Single crystal X-ray diffraction analysis to determine precise atomic structures.
Main Results:
- Successful synthesis of two new Au-Pt alloy nanoclusters: [Au24Pt(TBBT)12(TDT)3]0 and [Au24Pt(TBBT)12(PDT)3]0.
- Structural analysis revealed distinct -Au(I)-SR-Au(I)- staple lengths and orientations compared to previous analogues.
- The new nanoclusters exhibited significantly enhanced HER activity, with [Au24Pt(TBBT)12(TDT)3]0 being 3.5 times more active and [Au24Pt(TBBT)12(PDT)3]0 being 4.9 times more active than reference catalysts.
Conclusions:
- Subtle variations in ligand structure and metal-ligand staple geometry profoundly influence the electrocatalytic performance of Au-Pt nanoclusters.
- The synthesized [Au24Pt(TBBT)12(TDT)3]0 and [Au24Pt(TBBT)12(PDT)3]0 represent highly efficient electrocatalysts for HER.
- This work provides insights into designing advanced Au-Pt nanocluster catalysts with tunable properties for energy conversion applications.
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