‘Accelerated’ Deactivation of Carbon Nitride Photocatalyst for Solar Hydrogen Evolution

Abstract Carbon nitride photocatalysts are among the most studied candidates for efficient solar hydrogen (H2) production due to their abundance of precursors, suitable bandgap, and visible light utilization. However, the polymeric nature of carbon nitride materials raises concerns regarding the self‐decomposition during photocatalytic redox processes. Yet, the operational stability of carbon nitride photocatalysts for solar H2 production remains under‐explored. Here we evaluate the photostability of carbon nitride photocatalysts with platinum (Pt) as the co‐catalyst for solar H2 evolution and significant deactivation of this photocatalyst is observed under'accelerated’ testing conditions. It is demonstrated that the detachment of the Pt co‐catalyst on the surface of carbon nitride is the major reason for this deactivation, which can be attributed to a synergistic effect of photo‐corrosion and mechanical stirring. The photo‐corrosion weakens the interfacial bonding between carbon nitride and Pt co‐catalyst, while continuous collisions from the mechanical stirring promote the detachment of co‐catalysts from the surface of carbon nitride. These understandings provide insights into the rational design of photocatalysts and photocatalytic systems for improved operational stability.