Selective Photocatalytic Dehydrogenation of Formic Acid on Graphite Carbon Nitride with Dual-Sited Cobalt and Platinum Cocatalysts
Hang Xu, Heng Zhao, Jian Xu, Mehdi Eisapour, Zechuan Yu, Hang Su, Yuan Li, Fujian Zhou, Jinguang Hu, Zhangxin Chen
Abstract
Photocatalytic hydrogen production from the selective dehydrogenation of liquid organic hydrogen carriers is emerging as a promising alternative for green hydrogen generation. In this work, graphite carbon nitride (CN)-based photocatalyst is rationally designed by photodeposition of cobalt oxide nanoparticles as the hole trapper for the deprotonation of formic acid (FA), while the photogenerated electrons collected by in situ photodeposited platinum (Pt) nanoparticles reduce these protons to produce sustainable hydrogen. As a result, the well-designed photocatalyst (Co-CN) exhibits excellent hydrogen evolution activity (9039 μmol/h/g) and >99.98% dehydrogenation selectivity. Besides, Co-CN shows great durability in the long-time cycling test. Density functional theory reveals the contribution of Pt and cobalt oxide on the deprotonation from O–H and C–H breakage, respectively. Technoeconomic analysis demonstrates the potential of this reaction system for scale-up application. This present work demonstrates a great example for green hydrogen production from dehydrogenation of liquid organic hydrogen carriers under a mild condition.