Generation of free hydrogen atoms in thermal reaction of ethane with AuNbO 3 + cluster cations

Li, Ya‐Ke; Meng, Junwei; He, Sheng‐Gui

doi:10.1016/j.ijms.2015.02.001

Cited by 12 publications

(5 citation statements)

References 72 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Studying individual active species confined on atomic clusters , that can be explored under isolated, controlled, and reproducible conditions has been recently demonstrated to be successful. The spin and charge effects on the reactivity of atomic oxygen radical anions (O •– ) on atomic clusters have been revealed. , The extraordinary activity of single noble metal atoms including Au 1 and Pt 1 on metal oxide clusters could also be discovered. , The investigations of the Au 1 -doped metal oxide clusters have demonstrated that the conversions of Au I –O into Au –I –M (M = Ti, Fe, Nb, Ce, and Al) species could drive CO oxidation, dihydrogen activation, and so on . However, possibly because Au III has a high standard reduction potential, the preparation of Au III onto metal oxide clusters was unsuccessful in the previous experiments , and the chemical bonding and reactivity of the important Au III species on metal oxide clusters have been unknown yet.…”

Section: Introductionmentioning

confidence: 99%

Gold(III) Mediated Activation and Transformation of Methane on Au₁-Doped Vanadium Oxide Cluster Cations AuV₂O₆⁺

Zhao

et al. 2016

J. Am. Chem. Soc.

Self Cite

View full text Add to dashboard Cite

Gold in the +III oxidation state (Au(III)) has been proposed as a promising species to mediate challenging chemical reactions. However, it is difficult to characterize the chemistry of individual Au(III) species in condensed-phase systems mainly due to the interference from the Au(I) counterpart. Herein, by doping Au atoms into gas-phase vanadium oxide clusters, we demonstrate that the Au(III) cation in the AuV2O6(+) cluster is active for activation and transformation of methane, the most stable alkane molecule, into formaldehyde under mild conditions. In contrast, the AuV2O6(+) cluster isomers with the Au(I) cation can only absorb CH4. The clusters were generated by laser ablation and mass selected to react with CH4, CD4, or CH2D2 in an ion trap reactor. The reactivity was characterized by mass spectrometry and quantum chemistry calculations. The structures of the reactant and product ions were identified by using collision-induced and 425 nm photo-induced dissociation techniques.

show abstract

Section: Introductionmentioning

confidence: 99%

Gold(III) Mediated Activation and Transformation of Methane on Au₁-Doped Vanadium Oxide Cluster Cations AuV₂O₆⁺

Zhao

et al. 2016

J. Am. Chem. Soc.

Self Cite

View full text Add to dashboard Cite

show abstract

“…The gas-phase studies of binary TM oxides containing vanadium, such as AlVO n + ( n = 3–4) and Au 2 VO n + ( n = 3–4), demonstrate their ability to selectively oxidize CO. Niobium being a homotope of vanadium may have similar chemical reactivity. Recently, the fast-flow reactor experiments under both mass-nonselective and mass-selective conditions have identified the reactivity of the gold-doped niobium oxide clusters toward hydrocarbon molecules. − Here we present a joint photoelectron velocity-map imaging spectroscopic and theoretical study on CO oxidation by the bridging oxygen in the heterodinuclear niobium–nickel monoxide anion during the consecutive CO adsorption progress.…”

mentioning

confidence: 99%

Ligand-Mediated Reactivity in CO Oxidation of Niobium–Nickel Monoxide Carbonyl Complexes: The Crucial Roles of the Multiple Adsorption of CO Molecules

Zhang

Wang

Liu

et al. 2019

J. Phys. Chem. Lett.

View full text Add to dashboard Cite

The heteronuclear metal oxide complexes are of great significance in heterogeneous catalytic oxidation of CO. However, previous studies are mainly focused on the composition of metal oxide, charge state, the support and the active oxygen species, with little attention paid to adsorbed CO ligands. Herein, the ligand-mediated reactivity in CO oxidation of niobium−nickel monoxide carbonyl complexes has been successfully identified. The NbNiO(CO) n − (n = 5−6) anions are determined to be Obridged complexes. In contrast, the NbNiO(CO) n − (n = 7−8) anions are characterized to be η 2 -CO 2 -tagged complexes. The crucial roles of the multiply adsorbed CO molecules that can facilitate not only the competitive binding with bridging oxygen atom to the transition metal centers but also the electron accumulation of transition metal atoms have been discovered. The fascinating results are of substantial importance to understand the mechanisms of CO oxidation over heteronuclear metal oxide under CO-rich feed condition.

show abstract

“…Additionally, the making and breaking of the Au−O and Au−V (Au−M) bonds is the driving force for the oxidation of H 2 by Au 2 VO 4 + and Au 2 VO 3 + , which is consistent with the oxidation of some small molecules by gold-containing heteronuclear oxide clusters, such as the oxidation of methane and ethane by AuNbO 3 + , 59,60 the oxidation of CO by AuAl 3 O 5 + , 52 Au-(TiO 2 ) y O z − (y = 2, 3; z = 1, 2), 56 and Au 2 VO x − (x = 3, 4). 44…”

mentioning

confidence: 60%

Consecutive H₂ Oxidation Mediated by Au₂VO₄⁺ Clusters

Zhou

et al. 2016

J. Phys. Chem. C

Self Cite

View full text Add to dashboard Cite

Laser-ablation generated gold–vanadium oxide cluster cations Au2VO x + (x = 3, 4) were mass-selected by a quadrupole mass filter and interacted with H2 in an ion trap reactor. The reactions were characterized by mass spectrometry and density functional theory calculations. The Au2VO4 + cluster can oxidize two H2 molecules consecutively to produce Au2VO3 + and then Au2VO2 +, the latter of which can react with one O2 molecule to regenerate Au2VO4 +. Therefore, a catalytic cycle for H2 oxidation by O2 mediated with the Au2VO2 + clusters can be proposed. The theoretical studies predict that the gold atoms in both Au2VO4 + and Au2VO3 + are the active adsorption sites and facilitate the heterolytic cleavage of H2 in collaboration with the separate O2– ions of the vanadium oxide support. The consecutively oxidative reactivity of Au2VO4 + is attributed to the activation and dissociation of the superoxide or peroxide species (O2 •– or O2 2–) into two reactive atomic oxygen species (O2–) with the promotional effect of gold atoms acting as electron donors. This study provides molecular-level insights into the elementary mechanisms of the H2 catalytic oxidation on the surface.

show abstract

Generation of free hydrogen atoms in thermal reaction of ethane with AuNbO 3 + cluster cations

Cited by 12 publications

References 72 publications

Gold(III) Mediated Activation and Transformation of Methane on Au₁-Doped Vanadium Oxide Cluster Cations AuV₂O₆⁺

Gold(III) Mediated Activation and Transformation of Methane on Au₁-Doped Vanadium Oxide Cluster Cations AuV₂O₆⁺

Ligand-Mediated Reactivity in CO Oxidation of Niobium–Nickel Monoxide Carbonyl Complexes: The Crucial Roles of the Multiple Adsorption of CO Molecules

Consecutive H₂ Oxidation Mediated by Au₂VO₄⁺ Clusters

Contact Info

Product

Resources

About

Generation of free hydrogen atoms in thermal reaction of ethane with AuNbO 3 + cluster cations

Cited by 12 publications

References 72 publications

Gold(III) Mediated Activation and Transformation of Methane on Au1-Doped Vanadium Oxide Cluster Cations AuV2O6+

Gold(III) Mediated Activation and Transformation of Methane on Au1-Doped Vanadium Oxide Cluster Cations AuV2O6+

Ligand-Mediated Reactivity in CO Oxidation of Niobium–Nickel Monoxide Carbonyl Complexes: The Crucial Roles of the Multiple Adsorption of CO Molecules

Consecutive H2 Oxidation Mediated by Au2VO4+ Clusters

Contact Info

Product

Resources

About

Gold(III) Mediated Activation and Transformation of Methane on Au₁-Doped Vanadium Oxide Cluster Cations AuV₂O₆⁺

Gold(III) Mediated Activation and Transformation of Methane on Au₁-Doped Vanadium Oxide Cluster Cations AuV₂O₆⁺

Consecutive H₂ Oxidation Mediated by Au₂VO₄⁺ Clusters