Abstract
The advancement of an effective hydrogen liberation tech-nology from liquid organic hydrogen carriers (LOHCs), such as cyclohexane and methylcyclohexane (MCH), holds significance in realizing a hydrogen-centric society. However, the attainment of homogeneous catalytic acceptorless dehydrogenation (CAD) characterized by elevated selectivity for thorough aromatization under mild conditions remains unrealized. In this study, a catalyst system, facilitated by a double hydrogen atom transfer (HAT) processes, has been devised for the CAD of inert cycloalkanes at ambient temperature under visible light irradiation. Through the synergistic utilization of tetrabutylammonium chloride (TBACl) and thiophosphoric acid (TPA) HAT catalysts, successful CAD with comprehensive aromatization has been accomplished with high functional group tolerance.