Cooperative hydrogen production and C−C coupling organic synthesis in one photoredox cycle

Abstract

Coupling hydrogen fuel production with selective oxidative organic synthesis in one cooperative manner offers a promising avenue to enable efficient utilization of photoexcited carriers to achieve sustainable chemistry. Herein, a new Mo2N/Mn0.3Cd0.7S/CoPi photocatalyst is reported for visible-light-driven hydrogen production paired with selectively oxidative CC bond formation. Mo2N acting as electron collectors and reduction sites are adsorbed on the Mn0.3Cd0.7S by interfacial Mo-S bond, while CoPi acting as hole collectors and active sites for oxidation reaction are deposited on Mo2N/Mn0.3Cd0.7S. Remarkably, the synergetic effect of Mo2N and CoPi dual cocatalysts results in the adjustable flexibility of switching benzaldehyde (BAD) production to CC coupling synthesis, thus exhibiting the high selectivity of CC coupling products. Mechanism studies indicate that the CC coupling reaction occurs through a free radical mechanism. The present work gives insight for achieving highly efficient C−C coupling synthesis with hydrogen evolution by loading dual cocatalysts.