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Activation of Methane and Ethane as Mediated by the Triatomic Anion HNbN − : Electronic Structure Similarity with a Pt Atom
Author(s) -
Ma JiaBi,
Xu LinLin,
Liu QingYu,
He ShengGui
Publication year - 2016
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201511507
Subject(s) - chemistry , density functional theory , electronic structure , triatomic molecule , catalysis , ion , atom (system on chip) , atomic orbital , computational chemistry , chemical physics , atomic physics , inorganic chemistry , molecule , organic chemistry , physics , electron , quantum mechanics , computer science , embedded system
Investigations of the intrinsic properties of gas‐phase transition metal nitride (TMN) ions represent one approach to gain a fundamental understanding of the active sites of TMN catalysts, the activities and electronic structures of which are known to be comparable to those of noble metal catalysts. Herein, we investigate the structures and reactivities of the triatomic anions HNbN − by means of mass spectrometry and photoelectron imaging spectroscopy, in conjunction with density functional theory calculations. The HNbN − anions are capable of activating CH 4 and C 2 H 6 through oxidative addition, exhibiting similar reactivities to free Pt atoms. The similar electronic structures of HNbN − and Pt, especially the active orbitals, are responsible for this resemblance. Compared to the inert NbN − , the coordination of the H atom in HNbN − is indispensable. New insights into how to replace noble metals with TMNs may be derived from this combined experimental/computational study.