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Platinum Graphene Catalytic Condenser for Millisecond Programmable Metal Surfaces
Tzia Ming Onn1,2, Sallye R Gathmann1,2, Silu Guo2
1Center for Programmable Energy Catalysis (CPEC), University of Minnesota, 421 Washington Ave. SE, Minneapolis, Minnesota55455, United States.
Journal of the American Chemical Society
|November 16, 2022
Summary
Researchers precisely controlled platinum nanocluster electron density using a catalytic condenser. This tuning significantly altered carbon monoxide binding energies, paving the way for programmable catalytic surface conditions.
Area of Science:
- Surface Science and Catalysis
- Nanomaterials and Nanotechnology
- Electrochemistry and Materials Science
Background:
- Precise control over metal atom electron density is crucial for advancing catalytic chemistry and surface reactions.
- Existing methods for tuning catalytic activity often lack fine control over electron density at active sites.
Purpose of the Study:
- To develop a method for precisely controlling the electron density of platinum nanoclusters.
- To investigate the impact of controlled electron density on catalytic surface reactions, specifically carbon monoxide binding.
- To demonstrate the feasibility of creating programmable surface conditions for catalysis.
Main Methods:
- Fabrication of a catalytic condenser device using platinum nanoclusters supported on graphene over a HfO2 dielectric and a p-type Si wafer.
- Application of applied potentials (±6 V) to induce electron or hole accumulation in platinum active sites.
- Characterization using density functional theory (DFT) for binding energy computation, temperature-programmed desorption (TPD), equilibrium surface coverage measurements, and impedance spectroscopy.
Main Results:
- Achieved charge densities exceeding 1% of an electron or hole per surface platinum atom.
- Demonstrated a significant change in carbon monoxide binding energy (up to 24 kJ mol⁻¹) with controlled charge condensation, consistent with experimental measurements.
- Impedance spectroscopy confirmed negligible loss in capacitance and charge accumulation at high frequencies (3000 Hz), indicating stable programmable surface conditions.
Conclusions:
- The catalytic condenser effectively enables precise, programmable control over the electron density of platinum nanoclusters.
- Tuning electron density significantly impacts the binding energy of adsorbates like carbon monoxide, offering a new route for catalyst optimization.
- This approach provides a pathway to achieve 'catalytic resonance' by dynamically controlling surface conditions at relevant frequencies.
