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This study sheds light on the cleavage and reorganization of C(sp3)H and CN bonds of carbodiimides in a three‐component reaction of terminal alkynes, sulfur, and carbodiimides by a combination of methods including 1) isolation and X‐ray analysis of six‐membered‐ring lithium species 2‐S, 2) trapping of the oxygen‐analogues (B‐O and D‐O) of both four‐membered‐ring intermediate B‐S and ring‐opening...
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