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Described herein is an effective and green reaction between diketones, amines and bio‐renewable glyoxal, affording a wide range of 2‐pyrrolin‐5‐ones and releasing water as the only byproduct. The reaction features step‐economy, high efficiency, mild conditions, broad substrate scope, hazardous waste avoiding and easy scale‐up. The further transformation between the products and aldehydes can be potentially...