Size‐Dependent Reactivity of Nano‐Sized Neutral Manganese Oxide Clusters toward Ethylene

Chen, Jiaojiao; Zhang, Ting; Zhang, Meiqi; Liu, Qingyu; Li, Xiaona; He, Sheng‐Gui

doi:10.1002/chem.201703745

Cited by 14 publications

(7 citation statements)

References 79 publications

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“…[23][24][25][26][27] By conducting investigations of metal cluster catalysis, extensive efforts have been made to improve the reaction activity, and it is recognized that the specific sizes and geometric/electronic structures of clusters are often crucial factors in determining the resulting mechanisms and reaction rates. [28][29][30][31][32][33] Also, the binding energies can fluctuate with increasing numbers of atoms, allowing clusters at a certain size to transform from a two-dimensional planar structure to a three-dimensional (3-D) structure (e.g., Pt 3 vs Pt 4 ), and occasionally leading to "magic" number species such as Al 13 − , Ag 13 − , and 12,[34][35][36] In many studies, clusters are supported on a selected substrate in order to evaluate the catalytic reactions in a practical way. The interaction between the metal clusters and support is a fundamental characteristic in heterogeneous catalysis and plays an essential role in elucidating the electronic structures, adsorption behavior, and catalytic activities.…”

Section: Introductionmentioning

confidence: 99%

Enhanced Catalysis of Pt ₃ Clusters Supported on Graphene for N–H Bond Dissociation

Cui¹,

Luo²,

Yao³

2019

CCS Chem

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We report an in-depth study of catalytic N–H bond dissociation with typical platinum clusters on graphene supports. Among all the pristine graphene- and defective graphene-supported Pt clusters of different sizes that were studied, the Pt 3/G cluster possesses the highest reactivity and lowest activation barriers for each step of N–H dissociation in the decomposition of ammonia. In analyzing the reaction coordinates and projected density of states of the outermost orbitals, we found that the standing triangular Pt 3 on graphene creates prominent Lewis acid/base pair sites, which accommodate the adsorption and subsequent dissociation of *NH x . In comparison, Pt 1 lacks complementary active sites (CAS), causing it to be adverse to nucleophilic reactions, and in contrast, the Pt 13 cluster has weakened interactions and depleted charge density from the support, resulting in the elimination of the CAS effect. A stable pyramid-structured Pt 4 also develops Lewis acid/base sites, especially on defective graphene, but the density of states is still lower than the stand-up Pt 3/G. These findings strongly demonstrate the importance and necessity of cluster active sites for catalytic reactions of polar molecules, novel three-atoms metal cluster catalysis, and the selectivity and catalytic performance in the designing of ammonia fuel cells.

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Section: Introductionmentioning

confidence: 99%

Enhanced Catalysis of Pt ₃ Clusters Supported on Graphene for N–H Bond Dissociation

Cui¹,

Luo²,

Yao³

2019

CCS Chem

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“…The VUV single photon ionization coupled with TOF-MS has been demonstrated to be essential for detecting neutral species . The reactivity of neutral oxide clusters of manganese, , cobalt, iron, , and vanadium ,, toward CO, C 2 H 4 , NH 3 , C 4 H 10 , and CH 3 OH has been studied in recent years. It was found that the products detected by VUV photoionization were generated directly from the reactions of neutral metal oxide clusters with small molecules.…”

Section: Discussionmentioning

confidence: 99%

Vacuum Ultraviolet Ionization-Induced Reaction of Neutral Au₂Al₂O₃ Clusters with Methane

et al. 2018

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Identification of molecular-level mechanisms of methane activation is very important in order to transform the most stable alkane molecule into valueadded chemicals. Herein, by employing a homemade time-of-flight mass spectrometer coupled with a vacuum ultraviolet (VUV) laser system, the reactions of neutral heteronuclear metal oxide clusters Au x Al y O z (x = 1, 2) with CH 4 have been investigated. The interesting channel of Au 2 Al 2 O 3 H + production was observed for the interaction of a Au 2 Al 2 O 3 cluster with CH 4 after VUV ionization, suggesting that the methyl radical was generated. Combined with the theoretical calculations, this study proposes that VUV ionization of the neutral adsorption complex (Au 2 Al 2 O 3 CH 4 ) creates an active cation (Au 2 Al 2 O 3 CH 4 + )* to induce C−H bond activation and the methyl radical formation. The photochemistry of this cluster study provides molecular-level insights into the interactions between methane and active sites in related photocatalytic processes.

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“…After single photon ionization, the cluster ions passed through the reflector and then were detected by a dual microchannel plate detector. Note that most of the metal oxide clusters have ionization energies below 10.5 eV; , thus, most of them can be ionized and detected.…”

Section: Methodsmentioning

confidence: 99%

Catalytic CO Oxidation by Gas-Phase Metal Oxide Clusters

Wang

Mou

et al. 2019

J. Phys. Chem. A

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Oxidation of CO into CO 2 is a prototypical reaction in heterogeneous catalysis and is one of the extensively studied reactions in the gas phase to explore the underlying mechanisms of related catalysis. In this Feature Article, we present and discuss our recent advances in the fundamental understanding of catalytic CO oxidation by O 2 mediated with heteronuclear metal oxide clusters (HMOCs) using state-of-the-art mass spectrometry and quantum chemistry calculations. The HMOCs can be considered as ideal models for active sites on mixed or oxide supported catalysts at a strictly molecular level. A concept of electronegativity-ladder effect was proposed to account for the enhanced reactivity of noble metal (NM) doped HMOCs, and then this effect was successfully extended in the design of NM-free HMOCs in catalytic CO oxidation by O 2 . The future directions and the challenges were also discussed.

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Size‐Dependent Reactivity of Nano‐Sized Neutral Manganese Oxide Clusters toward Ethylene

Cited by 14 publications

References 79 publications

Enhanced Catalysis of Pt ₃ Clusters Supported on Graphene for N–H Bond Dissociation

Enhanced Catalysis of Pt ₃ Clusters Supported on Graphene for N–H Bond Dissociation

Vacuum Ultraviolet Ionization-Induced Reaction of Neutral Au₂Al₂O₃ Clusters with Methane

Catalytic CO Oxidation by Gas-Phase Metal Oxide Clusters

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Size‐Dependent Reactivity of Nano‐Sized Neutral Manganese Oxide Clusters toward Ethylene

Cited by 14 publications

References 79 publications

Enhanced Catalysis of Pt 3 Clusters Supported on Graphene for N–H Bond Dissociation

Enhanced Catalysis of Pt 3 Clusters Supported on Graphene for N–H Bond Dissociation

Vacuum Ultraviolet Ionization-Induced Reaction of Neutral Au2Al2O3 Clusters with Methane

Catalytic CO Oxidation by Gas-Phase Metal Oxide Clusters

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Resources

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Enhanced Catalysis of Pt ₃ Clusters Supported on Graphene for N–H Bond Dissociation

Enhanced Catalysis of Pt ₃ Clusters Supported on Graphene for N–H Bond Dissociation

Vacuum Ultraviolet Ionization-Induced Reaction of Neutral Au₂Al₂O₃ Clusters with Methane