Electrocatalytic Energy Release of Norbornadiene‐Based Molecular Solar Thermal Systems: Tuning the Electrochemical Stability by Molecular Design

Language
en
Document Type
Article
Issue Date
2023-04-21
First published
2022-12-20
Issue Year
2022
Authors
Franz, Evanie
Krappmann, Daniel
Fromm, Lukas
Luchs, Tobias
Görling, Andreas
Hirsch, Andreas
Brummel, Olaf
Libuda, Jörg
Editor
Publisher
Wiley-VCH GmbH
Abstract

Abstract Molecular solar thermal (MOST) systems, such as the norbornadiene/quadricyclane (NBD/QC) couple, combine solar energy conversion, storage, and release in a simple one‐photon one‐molecule process. Triggering the energy release electrochemically enables high control of the process, high selectivity, and reversibility. In this work, the influence of the molecular design of the MOST couple on the electrochemically triggered back‐conversion reaction was addressed for the first time. The MOST systems phenyl‐ethyl ester‐NBD/QC (NBD1/QC1) and p‐methoxyphenyl‐ethyl ester‐NBD/QC (NBD2/QC2) were investigated by in‐situ photoelectrochemical infrared spectroscopy, voltammetry, and density functional theory modelling. For QC1, partial decomposition (40 %) was observed upon back‐conversion and along with a voltammetric peak at 0.6 Vfc, which was assigned primarily to decomposition. The back‐conversion of QC2, however, occurred without detectable side products, and the corresponding peak at 0.45 Vfc was weaker by a factor of 10. It was concluded that the electrochemical stability of a NBD/QC couple is easy tunable by simple structural changes. Furthermore, the charge input and, therefore, the current for the electrochemically triggered energy release is very low, which ensures a high overall efficiency of the MOST system.

Journal Title
ChemSusChem
Volume
15
Issue
24
Citation
ChemSusChem 15.24 (2022): e202201483. <https://chemistry-europe.onlinelibrary.wiley.com/doi/10.1002/cssc.202201483>
Zugehörige ORCIDs