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How Hot Electron Generation at the Solid-Liquid Interface Is Different from the Solid-Gas Interface.

Si Woo Lee1,2, Heeyoung Kim2, Jeong Young Park2

  • 1Department of Chemistry Education, Korea National University of Education (KNUE), Chungbuk 28173, Republic of Korea.

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|March 17, 2023
PubMed
Summary
This summary is machine-generated.

Researchers discovered that hot electron excitation during chemical reactions is ~100 times more efficient at solid-liquid interfaces than solid-gas interfaces. This finding is crucial for understanding energy dissipation in catalysis.

Keywords:
catalytic nanodiodechemical energy conversionchemicurrenthot electronhydrogen peroxide decompositionsolid−liquid interface

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Area of Science:

  • Surface science
  • Catalysis
  • Physical chemistry

Background:

  • Exothermic chemical reactions on metal catalysts generate hot electrons via energy dissipation.
  • This phenomenon occurs at both solid-gas and solid-liquid interfaces.
  • Comparative operando studies directly comparing these interfaces are lacking.

Purpose of the Study:

  • To conduct a comparative operando study of hot electron excitation at solid-gas and solid-liquid interfaces.
  • To investigate the role of electronically nonadiabatic interactions in these processes.
  • To quantify the efficiency of hot electron generation in different phases.

Main Methods:

  • Utilized in situ techniques to monitor energy dissipation as chemicurrent.
  • Employed a platinum on n-type silicon (Pt/n-Si) nanodiode sensor.
  • Studied the decomposition of hydrogen peroxide (H2O2) in both gas and liquid phases.

Main Results:

  • Observed the generation of hot electrons in both gas and liquid phases during H2O2 decomposition.
  • Found that the efficiency of reaction-induced hot electron excitation was approximately 100 times higher at the solid-liquid interface compared to the solid-gas interface.
  • Correlated chemicurrent signals with oxygen evolution rates in both phases.

Conclusions:

  • The efficiency of hot electron excitation is significantly enhanced in the liquid phase.
  • An ionic layer at the solid-liquid interface lowers the potential barrier for hot electron transfer, boosting excitation.
  • This study provides critical insights into interfacial charge dynamics in catalytic reactions.