期刊
CHEMSUSCHEM
卷 15, 期 24, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202201483
关键词
electrochemistry; energy storage; photochemistry; photoswitches; solar thermal fuels
资金
- Deutsche Forschungsgemeinschaft (DFG) [392607742, 391585168]
- DFG [SFB 1452, 214951840, 453560721, 431733372, 322419553, FOR 1878]
- German Federal ministry of Education and Research (BMBF) [05 K19WE1]
- Bavarian ministry of Economic Affairs, Regional Development and Energy
- Projekt DEAL
This study investigated the influence of molecular design on the electrochemically triggered back-conversion reaction in MOST systems for the first time, showing that the electrochemical stability of a NBD/QC couple can be easily tuned by simple structural changes. Furthermore, the low charge input and current for the electrochemically triggered energy release ensure a high overall efficiency of the MOST system.
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 V-fc, which was assigned primarily to decomposition. The back-conversion of QC2, however, occurred without detectable side products, and the corresponding peak at 0.45 V-fc 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.
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