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A Gauss’s law analysis of redox active adsorbates on semiconductor electrodes: The charging and faradaic currents are not independent

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Significance Several strategies for low-cost solar energy conversion/storage systems are based upon redox-active molecules on semiconductor electrodes. Understanding charge transfer between such molecules and semiconductors is crucial for next-generation energy… Click to show full abstract

Significance Several strategies for low-cost solar energy conversion/storage systems are based upon redox-active molecules on semiconductor electrodes. Understanding charge transfer between such molecules and semiconductors is crucial for next-generation energy technologies. However, the immense difficulty in untangling the device physics, electrostatics, and chemical kinetics involved in the current-potential responses of these systems has been a long-standing challenge. In this work, we discovered a method for analyzing such data quantitatively and comprehensively. In doing so, we discovered an aspect of these systems that has been overlooked for more than a half century. Specifically, the act of passing one electron between the semiconductor and an adsorbed molecule can affect the ability to move the next electron to/from another adsorbed molecule.

Keywords: analysis redox; active adsorbates; redox active; law analysis; semiconductor electrodes; gauss law

Journal Title: Proceedings of the National Academy of Sciences of the United States of America
Year Published: 2022

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