Molecular photoswitches of norbornadiene (NBD) derivatives have been effectively applied in molecular solar-thermal energy storage (MOST) by photoisomerization of NBD to a quadricyclane (QC) state. However, a challenge of the NBD-based MOST system is the lack of a reversible two-way photoswitching process, limiting conversion from QC to thermal and catalytic methods. Here we design a series of NBD derivatives with a combination of acceptor and donor units to achieve two-way photoswitching, which can optically release energy by back-conversion from QC to NBD. Highly efficient photoconversion yields from NBD to QC and QC to NBD are up to 99% and 82%, respectively. The energy storage density of two-way photoswitching NBD is up to 312 J g-1 and optically controlled two-way photoswitching devices are demonstrated for the first time both in flow and in thin films, which illustrate a promising approach for fast and robust energy release in both solution and solid state.
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