Liberation of three dihydrogens from two ethene molecules as mediated by the tantalum nitride anion cluster TaN at room temperature.

The reactivity of gas-phase cluster anions TaN with CH under thermal collision conditions was studied by mass spectrometry in conjunction with density functional theory calculations. The full dehydrogenation of the CH molecule was observed, with the formation of two dihydrogen molecules. Interestingly, the two carbon atoms originating from the first CH molecule are used to construct another cluster TaNC, which can activate one more CH releasing one H molecule. Therefore, three dihydrogen molecules are liberated from two ethene molecules in the overall reaction. The full dehydrogenation of CH by gas-phase anions as well as the structure and reactivity of M-N-C (M: transition metal) cluster is reported for the first time. The properties of TaN and TaNC elucidated herein are of use in providing fundamental information that is necessary to tailor the design of new and effective catalysts by applying the related materials.