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Published on: July 27, 2018
Chemistry of fast electrons
Sergey N Maximoff1, Martin P Head-Gordon
1Department of Chemistry, University of California, and Chemical Science Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA. maximoff@berkeley.edu
Summary
Chemicurrents are electron fluxes from chemical reactions on metal surfaces. This study links chemicurrents to surface chemistry via electron localization and delocalization during reactions, revealing a power-law relationship with adsorption heat.
Area of Science:
- Surface Science
- Physical Chemistry
- Materials Science
Background:
- Chemicurrents are defined as fast electron fluxes generated by chemical reactions on metal surfaces.
- Understanding the relationship between surface chemistry and chemicurrents is crucial for catalysis and electronics.
Purpose of the Study:
- To elucidate the relationship between chemicurrents and surface chemistry.
- To investigate the mechanisms governing chemicurrent generation in catalytic reactions.
Main Methods:
- Combined top-down phenomenology and bottom-up atomic-scale modeling.
- Detailed examination of catalytic CO oxidation as a model system.
- Analysis of electron localization/delocalization during reduction and oxidation reactions.
Main Results:
- Identified three key processes: electron localization (Red), electron delocalization (Ox), and relaxation (Rel).
- Determined that CO2 reactive desorption dominates the chemicurrent due to its long-range and fast electron excitation.
- Established a power-law relationship (exponent 2.66) between chemicurrent yield and heat of adsorption.
Conclusions:
- The chemicurrent yield is dependent on the desorption process universality class and threshold distribution.
- The findings are applicable to various oxidation-reduction reactions on high work function metal surfaces.
- This work provides a fundamental understanding of electron transfer dynamics in surface chemistry.
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