Methane Activation by Tantalum Carbide Cluster Anions Ta2C4().

Title Methane Activation by Tantalum Carbide Cluster Anions Ta2C4().
Authors H.F. Li; Y.X. Zhao; Z. Yuan; Q.Y. Liu; Z.Y. Li; X.N. Li; C.G. Ning; S.G. He
Journal J Phys Chem Lett
DOI 10.1021/acs.jpclett.6b02568

Methane activation by transition metals is of fundamental interest and practical importance, as this process is extensively involved in the natural gas conversion to fuels and value-added chemicals. While single-metal centers have been well recognized as active sites for methane activation, the active center composed of two or more metal atoms is rarely addressed and the detailed reaction mechanism remains unclear. Here, by using state-of-the-art time-of-flight mass spectrometry, cryogenic anion photoelectron imaging spectroscopy, and quantum-chemical calculations, the cooperation of the two Ta atoms in a dinuclear carbide cluster Ta2C4(-) for methane activation has been identified. The C-H bond activation takes place predominantly around one Ta atom in the initial stage of the reaction and the second Ta atom accepts the delivered H atom from the C-H bond cleavage. The well-resolved vibrational spectra of the cryogenically cooled anions agree well with theoretical simulations, allowing the clear characterization of the structure of Ta2C4(-) cluster. The reactivity comparison between Ta2C4(-) cluster and the carbon-less analogues (Ta2C3(-) and Ta2C2(-)) demonstrated that the cooperative effect of the two metal atoms can be well tuned by the carbon ligands in terms of methane activation and transformation.

Citation H.F. Li; Y.X. Zhao; Z. Yuan; Q.Y. Liu; Z.Y. Li; X.N. Li; C.G. Ning; S.G. He.Methane Activation by Tantalum Carbide Cluster Anions Ta2C4().. J Phys Chem Lett. 2017;8(3):605610. doi:10.1021/acs.jpclett.6b02568

Related Elements


See more Tantalum products. Tantalum (atomic symbol: Ta, atomic number: 73) is a Block D, Group 5, Period 6 element with an atomic weight of 180.94788. Tantalum Bohr ModelThe number of electrons in each of tantalum's shells is [2, 8, 18, 32, 11, 2] and its electron configuration is [Xe] 4f14 5d3 6s2. The tantalum atom has a radius of 146 pm and a Van der Waals radius of 217 pm. High Purity (99.999%) Tantalum (Ta) MetalTantalum was first discovered by Anders G. Ekeberg in 1802 in Uppsala, Sweden however, it was not until 1844 when Heinrich Rose first recognized it as a distinct element. In its elemental form, tantalum has a grayish blue appearance. Tantalum is found in the minerals tantalite, microlite, wodginite, euxenite, and polycrase. Due to the close relation of tantalum to niobium in the periodic table, Tantalum's name originates from the Greek word Tantalos meaning Father of Niobe in Greek mythology.

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