The applications of electron spin resonance (ESR) to carbonaceous materials are reviewed. The stable paramagnetic species observed in the products of low-temperature pyrolysis are odd-alternate neutral free radicals, whereas the unpaired spins of higher temperature carbons and graphites are primarily conduction electrons. The variety of ESR properties and phenomena requires special attention to techniques of measurement and interpretations of results. The relevance to the carbonization process of the free radicals observed by ESR is also discussed.

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