As the world faces rising challenges from climate change and plastic pollution, science is searching for sustainable ways to produce everyday materials using renewable energy and environmentally friendly processes. This project responded to that challenge by developing a new solar-powered method to create diphenyl carbonate (DPC), a key building block in the production of polycarbonate plastics, commonly used in electronics, lenses, and medical devices. Traditionally, DPC is produced using toxic chemicals like phosgene, which poses health and environmental risks. This project instead explored an innovative and greener route: using carbon dioxide (CO2) and phenol, a common industrial feedstock, to produce DPC under solar light. By converting waste CO2 into valuable materials, the project aligned with Europe’s sustainability goals and circular economy strategies. The scientific goal was to design new photocatalytic materials that can perform two separate chemical reactions at once: reducing CO2 to carbon monoxide (CO*) and oxidizing phenol to phenoxy radicals (PhO•). These reactive intermediates are then coupled together to form DPC.
In this project, we aimed at two main objectives:
1. Engineering halide perovskites (HPs) with tailored band structures and controlled surface defects to anchor palladium (Pd) clusters or single atoms, creating porous hybrid materials with enhanced sunlight absorption and photocatalytic activity.
2. Demonstrating solar-mediated formation of key intermediates, including phenoxy radicals (PhO•) and carbon monoxide (CO*) from phenol oxidation and CO2 reduction, enabling tandem diphenyl carbonate (DPC) synthesis.
3. Uncovering the reaction mechanism through advanced spectroscopic tools and control experiments, identifying intermediate species and charge-transfer pathways to provide insights into the photocatalytic transformation reactions.
The innovation of this work lies not only in developing a cleaner, safer pathway for DPC production, but also in pioneering a new class of photocatalytic materials, single-atom catalyst (SAC) decorated halide perovskites (Figure 1). This unexplored combination has great potential in solar chemical synthesis and could be extended to other reactions. By bridging material science, green chemistry, and solar energy conversion, the project offers a blueprint for replacing fossil-fuel-based production processes with cleaner, sunlight-powered alternatives advancing both scientific understanding and sustainability goals.
