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Single-Atom Doping at the Molecule-Metal Interface: How Rh Affects Surface Explosion Kinetics.

Avery S Daniels1, Andrew J Gellman2, E Charles H Sykes1

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Summary
This summary is machine-generated.

Adding rhodium (Rh) atoms to a copper (Cu) surface dramatically alters tartaric acid (TA) decomposition. Rh accelerates both initiation and explosive decomposition, enabling control over these surface reactions at lower temperatures.

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Area of Science:

  • Surface chemistry and catalysis
  • Chemical kinetics
  • Materials science

Background:

  • Controlling interfacial reactions is crucial in atmospheric, environmental, biological chemistry, catalysis, and corrosion.
  • Tartaric acid (TA) decomposition on Cu(100) displays autocatalytic kinetics with a slow initiation followed by rapid decomposition ('surface explosions').
  • These reactions are highly sensitive to initial conditions, necessitating studies on how reactive atom placement impacts kinetics.

Purpose of the Study:

  • To investigate the influence of catalytically active rhodium (Rh) atoms on the surface reaction kinetics of tartaric acid (TA) decomposition.
  • To understand how the placement of Rh atoms (at or above the molecule-metal interface) affects TA decomposition rates and mechanisms on Cu(100).

Main Methods:

  • Utilized temperature-programmed reaction (TPR) experiments to study TA decomposition on modified Cu(100) surfaces.
  • Compared TA decomposition on Rh-embedded (TA/Rh/Cu) and Rh-atop (Rh/TA/Cu) surfaces with bare Cu(100).
  • Employed isothermal TPR analysis to determine initiation and explosion rate constants.

Main Results:

  • Rhodium atoms, whether embedded in or placed atop the TA layer on Cu(100), significantly reduced the decomposition temperature.
  • Both initiation (k_init) and explosion (k_exp) rate constants for TA decomposition were enhanced by the presence of Rh.
  • Isothermal TPR analysis confirmed Rh's acceleration of both kinetic steps, facilitating explosive decomposition at lower temperatures.

Conclusions:

  • Both initiation and explosive decomposition steps of TA occur at the metal-molecule interface.
  • Rhodium's presence at the interface accelerates these interfacial reactions.
  • Small amounts of reactive elements can effectively control nonlinear kinetic processes at surfaces.