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Controlled Shell and Kernel Modifications of Atomically Precise Pd/Ag Superatomic Nanoclusters.

Yu-Rong Ni1, Michael N Pillay1, Tzu-Hao Chiu1

  • 1Department of Chemistry, National Dong Hwa University, No. 1, Sec 2, Da Hsueh Rd., Hualien, 97401, Taiwan, R.O.C.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|March 10, 2023
PubMed
Summary
This summary is machine-generated.

The first 8-electron palladium/silver (Pd/Ag) superatomic alloys featuring an interstitial hydride were synthesized. These novel Pd/Ag superatomic alloys demonstrate catalytic activity for 4-nitrophenol reduction.

Keywords:
atomically precise nanoclustersdithiophosphatepalladium hydridessuperatoms

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Area of Science:

  • Superatomic Chemistry
  • Nanomaterials Synthesis
  • Catalysis

Background:

  • Superatomic alloys mimic atoms with unique electronic and structural properties.
  • Palladium and silver (Pd/Ag) clusters are of interest for their catalytic potential.
  • The role of interstitial species in superatomic cluster stability and properties is underexplored.

Purpose of the Study:

  • To synthesize and characterize novel 8-electron Pd/Ag superatomic alloys.
  • To investigate the influence of interstitial hydrides on superatomic electron counts and structures.
  • To explore the photophysical properties and catalytic applications of these new materials.

Main Methods:

  • Synthesis of [PdHAg19(dtp)12] (1) and [PdHAg20(dtp)12]+ (2) via controlled addition of silver atoms.
  • Characterization using multinuclear variable-temperature NMR spectroscopy to determine isomer distributions.
  • Photophysical measurements (emission lifetime) and catalytic activity testing (4-nitrophenol reduction).

Main Results:

  • Successfully synthesized the first 8-electron Pd/Ag superatomic alloys with interstitial hydrides.
  • Demonstrated the formation of 2 from 1 through targeted silver atom addition.
  • Observed luminescence in [PdAg21(dtp)12]+ (3) with a lifetime of 200 μs, while 1 and 2 are non-emissive.
  • Showcased the catalytic reduction of 4-nitrophenol by all synthesized clusters at room temperature.

Conclusions:

  • The interstitial hydride plays a crucial role in the 8-electron superatomic configuration of Pd/Ag clusters.
  • The synthesized Pd/Ag superatomic alloys exhibit tunable properties and potential as room-temperature catalysts.
  • This work expands the scope of superatomic cluster chemistry and their functional applications.