Thermal Methane Activation by La6O10− Cluster Anions

Meng, Junwei; Deng, Xiaojiao; Li, Ziyu; He, Sheng‐Gui; Zheng, Wei‐Jun

doi:10.1002/chem.201400218

Cited by 35 publications

(35 citation statements)

References 44 publications

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“…Gas‐phase studies of methane activation by metal atoms and clusters have provided insight into methane functionalization at the molecular level . In the case of platinum the reactivities of its cationic, neutral, and anionic atoms and clusters with methane have been widely investigated .…”

Section: Figurementioning

confidence: 99%

Selective Activation of the C−H Bond in Methane by Single Platinum Atomic Anions

et al. 2019

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Mass spectrometric analysis of the anionic products of interaction between platinum atomic anions,P t À ,a nd methane,CH 4 and CD 4 ,inacollision cell shows the preferred generation of [PtCH 4 ] À and [PtCD 4 ] À complexes and al ow tendency toward dehydrogenation. [PtCH 4 ] À is shown to be H À Pt À CH 3 À by as ynergy between anion photoelectron spectroscopya nd quantum chemical calculations,i mplying the rupture of as ingle CÀHb ond. The calculated reaction pathway accounts for the observed selective activation of methane by Pt À .T his study presents the first example of methane activation by as ingle atomic anion.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under https://doi.

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Section: Figurementioning

confidence: 99%

Selective Activation of the C−H Bond in Methane by Single Platinum Atomic Anions

et al. 2019

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“…[4,22,23] It was reported that the anions are mostly inert or react very slowly with methane. [4,22,23] It was reported that the anions are mostly inert or react very slowly with methane.…”

mentioning

confidence: 99%

“…Oxide cluster anions are usually inert with methane and it has been only recently identified that La 6 O 10 À and La 8 O 13 À anions can activate CH 4 through the OC À centers to generate CH 3 [Reaction (1)] under thermal collision conditions whereas the reaction efficiencies are quite low (F = 0.02-0.03 %), [22] in sharp contrast to the good efficiency of (7.0 AE 3.5) % for PtAl 2 O 4 À with CH 4 . This also implies that methane activation by PtAl 2 O 4 À follows a different mechanism.…”

mentioning

confidence: 99%

Thermal Methane Conversion to Formaldehyde Promoted by Single Platinum Atoms in PtAl₂O₄⁻ Cluster Anions

Zhao

Yuan

et al. 2014

Angewandte Chemie

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Identification and mechanistic study of thermal methane conversion mediated by gas-phase species is important for finding potentially useful routes for direct methane transformation under mild conditions. Negatively charged oxide species are usually inert with methane. This work reports an unexpected result that the bi-metallic oxide cluster anions PtAl 2 O 4 À can transform methane into a stable organic compound, formaldehyde, with high selectivity. The clusters are prepared by laser ablation and reacted with CH 4 in an ion trap reactor. The reaction is characterized by mass spectrometry and density functional theory calculations. It is found that platinum rather than oxygen activates CH 4 at the beginning of the reaction. The Al 2 O 4 À moiety serves as the support of Pt atom and plays important roles in the late stage of the reaction. A new mechanism for selective methane conversion is provided and new insights into the surface chemistry of single Pt atoms may be obtained from this study.

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“…178 The two cluster anions can abstract one hydrogen atom from methane to generate CH 3 178 The two cluster anions can abstract one hydrogen atom from methane to generate CH 3…”

Section: Reaction With Organic Substratesmentioning

confidence: 99%

Reactions of metal cluster anions with inorganic and organic molecules in the gas phase

et al. 2016

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The study of gas phase ion-molecule reactions by state-of-the-art mass spectrometric experiments in conjunction with quantum chemistry calculations offers an opportunity to clarify the elementary steps and mechanistic details of bond activation and conversion processes. In the past few decades, a considerable number of publications have been devoted to the ion-molecule reactions of metal clusters, the experimentally and theoretically tractable models for the active phase of condensed phase systems. The focus of this perspective concerns progress on activation and transformation of important inorganic and organic molecules by negatively charged metal clusters. The metal cluster anions cover bare metal clusters as well as ligated systems with oxygen, carbon, and nitrogen, among others. The following important issues have been summarized and discussed: (i) dependence of chemical reactivity and selectivity on cluster structures and sizes, metals and metal oxidation states, odd-even electron numbers, etc. and (ii) effects of doping, ligation, and pre-adsorption on the reactivity of metal clusters toward rather inert molecules.

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Thermal Methane Activation by La₆O₁₀⁻ Cluster Anions

Cited by 35 publications

References 44 publications

Selective Activation of the C−H Bond in Methane by Single Platinum Atomic Anions

Selective Activation of the C−H Bond in Methane by Single Platinum Atomic Anions

Thermal Methane Conversion to Formaldehyde Promoted by Single Platinum Atoms in PtAl₂O₄⁻ Cluster Anions

Reactions of metal cluster anions with inorganic and organic molecules in the gas phase

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Thermal Methane Activation by La6O10− Cluster Anions

Cited by 35 publications

References 44 publications

Selective Activation of the C−H Bond in Methane by Single Platinum Atomic Anions

Selective Activation of the C−H Bond in Methane by Single Platinum Atomic Anions

Thermal Methane Conversion to Formaldehyde Promoted by Single Platinum Atoms in PtAl2O4− Cluster Anions

Reactions of metal cluster anions with inorganic and organic molecules in the gas phase

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Thermal Methane Activation by La₆O₁₀⁻ Cluster Anions

Thermal Methane Conversion to Formaldehyde Promoted by Single Platinum Atoms in PtAl₂O₄⁻ Cluster Anions