Decoupling Kinetics and Thermodynamics of Interfacial Catalysis at a Chemically Modified Black Silicon Semiconductor Photoelectrode

Caitlin Hanna, Ryan Pekarek, Elisa Miller, Jenny Yang, Nathan Neale

Research output: Contribution to journalArticlepeer-review

8 Scopus Citations

Abstract

Understanding the interplay between the kinetics of interfacial catalytic reactions and the thermodynamics of an underlying semiconductor electrode is imperative for rational construction of efficient photoelectrocatalytic systems. Current understanding of the thermodynamic effects of molecular catalyst attachment to semiconductor electrodes is limited. We report the immobilization of a molecular cobalt bis(benzenedithiolate) proton reduction catalyst onto nanoporous black silicon (b-Si) electrodes through π-πinteractions with a series of aromatic molecules covalently attached to the surface. Intensity-modulated high-frequency resistivity and linear sweep voltammetry measurements are used to show that the kinetics of proton reduction are decoupled from the thermodynamic properties of the underlying b-Si photoelectrode.

Original languageAmerican English
Pages (from-to)1848-1855
Number of pages8
JournalACS Energy Letters
Volume5
Issue number6
DOIs
StatePublished - 12 Jun 2020

Bibliographical note

Publisher Copyright:
Copyright © 2020 American Chemical Society.

NREL Publication Number

  • NREL/JA-5900-77356

Keywords

  • catalysis
  • catalysts
  • electrodes
  • kinetics
  • solar-photochemistry
  • thermodynamic properties

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