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Addition of CO to a tetrametallic magnesium hydride cluster results in both carbon‐carbon bond formation and deoxygenation to generate an acetaldehyde enolate [C2OH3]− which remains coordinated to the cluster. To the best of our knowledge, this is the first example of formation of an isolable complex containing an [C2OH3]− fragment from reaction of CO with a metal hydride, and the first example of...