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Rhodium‐catalyzed acrylate synthesis from CO2 and ethylene was accomplished by using a guanidine‐based NCN pincer ligand. The repulsion between pπ‐electron of guanidine sidearms and occupied dπ orbital of rhodium center raised the level of d‐electrons close to those of formerly known d8‐ruthenium catalyst, thereby promoting the metallalactone formation from carbon dioxide and ethylene. This work fills...