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With the help of density functional theory (DFT) calculations, we theoretically investigated and rationalized the controlled metathesis reactions of methylruthenium complex trans‐[Ru(CH3)2(dmpe)2] [dmpe = 1,2‐bis(dimethylphosphanyl)ethane] (A) with terminal acetylenes. On the basis of the mechanistic study, two important issues related to the generation of mono‐ and bis‐acetylido Ru complexes have...
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