Carbide Dihydrides: Carbonaceous Species Identified in Ta4+‐Mediated Methane Dehydrogenation

作者：Jozef Lengyel, Nikita Levin, Frank J. Wensink, Olga V. Lushchikova, R. N. Barnett, Uzi Landman, Ueli Heiz, Joost M. Bakker, Martin Tschurl · 发表于：Angewandte Chemie International Edition · 年份：2020 · DOI：10.1002/anie.202010794 · 被引用次数：22 · 研究领域：Catalytic Processes in Materials Science、Catalysis and Oxidation Reactions、Asymmetric Hydrogenation and Catalysis

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.