Carbide Dihydrides: Carbonaceous Species Identified in Ta<sub>4</sub><sup>+</sup>‐Mediated Methane Dehydrogenation
Jozef Lengyel, Nikita Levin, Frank J. Wensink, Olga V. Lushchikova, R. N. Barnett, Uzi Landman, Ueli Heiz, Joost M. Bakker, Martin Tschurl
Abstract
Abstract The products of methane dehydrogenation by gas‐phase Ta 4 + clusters are structurally characterized using infrared multiple photon dissociation (IRMPD) spectroscopy in conjunction with quantum chemical calculations. The obtained spectra of [4Ta,C,2H] + reveal a dominance of vibrational bands of a H 2 Ta 4 C + carbide dihydride structure over those indicative for a HTa 4 CH + carbyne hydride one, as is unambiguously verified by studies employing various methane isotopologues. Because methane dehydrogenation by metal cations M + typically leads to the formation of either MCH 2 + carbene or HMCH + carbyne hydride structures, the observation of a H 2 MC + carbide dihydride structure implies that it is imperative to consider this often‐neglected class of carbonaceous intermediates in the reaction of metals with hydrocarbons.