Nitroxides are widely used as probes and polarization transfer agents in spectroscopy and imaging.These applications require high stability towards reducing biological environments, as well as beneficial relaxation properties. Closed spirocyclohexyl nitroxides exhibit a dramatically improved stability towards reduction by ascorbate, while maintaining long relaxation times in EPR spectroscopy. This dataset contains raw files and analysis reports of 1HNMR, 13CNMR, HRMS, FTIR of all compounds synthesized for and used in work: Conformational tuning improves the stability of spirocyclic nitroxides with long paramagnetic relaxation times. Moreover, for nitroxides raw files of X-band CW-EPR spectra, kinetic runs based on CW-EPR spectra and Q-band EPR relaxation measurements are included. Dataset is completed with X-ray crystallography CIF files and reports, as well as all optimized geometries for discussed conformers
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