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This effect enables an efficient inverse Stone\u2013Wales rearrangement at temperatures as low as 250 \u00b0C for potassium-, rubidium-, and cesium-doped systems. In contrast, lithium and sodium doping exclusively promote cyclodehydrogenation at cove regions. Supported by density functional theory, we propose a mechanistically consistent pathway and report the isolation and characterization of key anionic intermediates by single-crystal X-ray diffraction, UV\u2013vis spectroscopy, and magnetometry. 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