Upcycling of Acid Waste Gases Using Asymmetric Atomic-Copper-Anchored Covalent Organic Framework Catalyst

Catalytic conversion of acid waste gases into value-added chemicals is crucial for sustainable carbon and sulfur utilization, and designing efficient and stable catalysts shows great significance in achieving this goal. Herein, we report an olefin-linked, bipyridine-functionalized COF with atomically dispersed Cu active sites (xCu@COF-PzBpy) that combines high specific surface area, robust stability, and an asymmetric Cu-N4 coordination geometry induced by the interlayer stress effect. The newly engineered Cu-N4 active centers demonstrate enhanced activation capability for both acid gases and epoxides, endowing xCu@COF-PzBpy with an exceptional catalytic performance for their upcycling under ambient conditions. This performance outperforms nearly all previously reported catalysts. Similarly, the high catalytic activities of xCu@COF-PzBpy can be extended to the COS and SO2 cycloaddition. No activity loss, Cu leaching, and/or aggregation were observed over 10 cycles. This work provides a new strategy for developing efficient and reusable catalysts for acid waste gas upcycling, addressing environmental challenges while enabling green and sustainable cycles.