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Species bearing unpaired electrons, including paramagnetic redox metal centres, surface defect centres, reactive oxygen species, adsorbed radical anions, are often involved in catalytic reactions. These species can be readily and thoroughly interrogated using Electron Paramagnetic Resonance (EPR) spectroscopy, providing information on the identity, chemical composition and even the dynamics of the centres themselves, thereby helping to elucidate the involvement of the radicals in the reaction cycles. This review will summarise and highlight the applications of EPR in heterogeneous, homogeneous, photocatalytic and microporous materials, all of which are of vital importance to the field of catalysis.

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