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Capturing Dynamic Core Reconstruction and Ligand Desorption of Atomically Precise Ag Nanoclusters with Machine

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Atomically precise silver nanoclusters (NCs) are promising electrocatalysts. Doping these NCs with other metals or elements significantly enhances their stability and structural evolution dynamics under electrochemical conditions, enabling better catalyst design.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Computational Chemistry

Background:

  • Atomically precise silver nanoclusters (NCs) protected by alkynyl ligands show potential as electrocatalysts for CO2 electroreduction.
  • Understanding the dynamic structural evolution of these NCs under electrochemical conditions is crucial but challenging due to limitations in experimental and traditional simulation techniques.

Purpose of the Study:

  • To elucidate the electrochemical structural evolution mechanisms of alkynyl-protected Ag15 NCs and their doped systems (Ag8Au7, Ag9Cu6, Ag14Cl).
  • To establish a quantitative correlation between electrochemical interface dynamics and doping effects for designing stable atomically precise catalysts.

Main Methods:

  • Developed a high-accuracy machine learning force field using a deep potential molecular dynamics (DPMD) scheme combined with multiscale constant potential simulations.
  • Performed nanosecond-level DPMD simulations to capture atomic-scale dynamic processes and electrochemical interface evolution.

Main Results:

  • Observed a transition from octahedral to disordered metal cores in all NCs, with partial or complete alkynyl ligand cleavage.
  • Dopants modulate NC stability by regulating ligand desorption pathways; Ag9Cu6 NC showed superior resistance due to robust Cu-C bonding.
  • Doping significantly affects the number of desorbed ligands and core ordering, with long-term simulations crucial for capturing interface dynamics.

Conclusions:

  • The study provides the first quantitative correlation between electrochemical interface dynamics and doping effects in atomically precise nanoclusters.
  • The findings offer a theoretical framework for designing highly stable and active atomically precise electrocatalysts through strategic doping.