Innovative two-dimensional porphyrin-integrated metal-organic frameworks for enhanced photocatalytic hydrogen peroxide generation in pure water

Abstract

In the quest for eco-friendly and efficient synthesis of hydrogen peroxide (H2O2), a chemical with extensive applications, photocatalytic production emerges as a promising clean technique. Metal-organic frameworks (MOFs), known for their exceptional porosity and geometric customizability, stand at the forefront of potential photocatalytic materials. Yet, the conventional three-dimensional topologies of MOFs pose a challenge, impeding the swift transit of photogenerated electrons and thereby curbing performance enhancements. In this vein, we have engineered novel 2D porphyrin-based MOFs, specifically Ce-TCPP and La-TCPP, utilizing diverse metal sources while maintaining a consistent topological framework. This design strategy streamlines the electron and hole transport pathways, thus elevating the photocatalytic activity. Delving into the structural nuances of these MOFs, our research unveiled that the photocatalytic activity experienced a marked shift upon altering the metal cluster types. Notably, La-TCPP, as an efficacious catalyst, demonstrated an H2O2 yield of 79.75 μmol/g/h in pure water, sans any sacrificial agents. Rigorous testing confirmed the robust stability of both MOFs. This study marks the inaugural design and synthesis of a single crystal structure of La-TCPP. By strategically varying metal cluster compositions, we have fine-tuned the architecture of two-dimensional MOFs. This approach sheds light on the intricate structure-activity relationship governing the photocatalytic synthesis of H2O2, paving the way for future advancements in the field.