Double-oxygen-atom transfer in reactions of CemO 2m+ (m=2-6) with C2H2

Xun Lei Ding; Xiao Nan Wu; Yan Xia Zhao; Jia Bi Ma; Sheng Gui He

doi:10.1002/cphc.201100216

Double-oxygen-atom transfer in reactions of Ce_mO _2m⁺ (m=2-6) with C₂H₂

Xun Lei Ding, Xiao Nan Wu, Yan Xia Zhao, Jia Bi Ma, Sheng Gui He^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

27 Citations (Scopus)

Abstract

Cerium oxide cluster cations (Ce_mO_n⁺, m=2-16; n=2m, 2m±1 and 2m±2) are prepared by laser ablation and reacted with acetylene (C₂H₂) in a fast-flow reactor. A time-of-flight mass spectrometer is used to detect the cluster distribution before and after the reactions. Reactions of stoichiometric Ce_mO _2m⁺ (m=2-6) with C₂H₂ produce Ce_mO_2m-2⁺ clusters, which indicates a "double-oxygen-atom transfer" reaction Ce_mO _2m⁺+C₂H₂→Ce_mO _2m-2⁺+(CHO)₂ (ethanedial). A single-oxygen-atom transfer reaction channel is also identified as Ce_mO _2m⁺+C₂H₂→Ce_mO _2m-1⁺+C₂H₂O (at least for m=2 and 3). Density functional theory calculations are performed to study reaction mechanisms of Ce₂O₄⁺+C₂H ₂, and the calculated results confirm that both the single- and double-oxygen-atom transfer channels are thermodynamically and kinetically favourable.

Original language	English
Pages (from-to)	2110-2117
Number of pages	8
Journal	ChemPhysChem
Volume	12
Issue number	11
DOIs	https://doi.org/10.1002/cphc.201100216
Publication status	Published - 1 Aug 2011
Externally published	Yes

Keywords

cerium
cluster compounds
density functional calculations
mass spectrometry
reaction mechanisms

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title = "Double-oxygen-atom transfer in reactions of CemO 2m+ (m=2-6) with C2H2",

abstract = "Cerium oxide cluster cations (CemOn+, m=2-16; n=2m, 2m±1 and 2m±2) are prepared by laser ablation and reacted with acetylene (C2H2) in a fast-flow reactor. A time-of-flight mass spectrometer is used to detect the cluster distribution before and after the reactions. Reactions of stoichiometric CemO 2m+ (m=2-6) with C2H2 produce CemO2m-2+ clusters, which indicates a {"}double-oxygen-atom transfer{"} reaction CemO 2m++C2H2→CemO 2m-2++(CHO)2 (ethanedial). A single-oxygen-atom transfer reaction channel is also identified as CemO 2m++C2H2→CemO 2m-1++C2H2O (at least for m=2 and 3). Density functional theory calculations are performed to study reaction mechanisms of Ce2O4++C2H 2, and the calculated results confirm that both the single- and double-oxygen-atom transfer channels are thermodynamically and kinetically favourable.",

keywords = "cerium, cluster compounds, density functional calculations, mass spectrometry, reaction mechanisms",

author = "Ding, {Xun Lei} and Wu, {Xiao Nan} and Zhao, {Yan Xia} and Ma, {Jia Bi} and He, {Sheng Gui}",

year = "2011",

month = aug,

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doi = "10.1002/cphc.201100216",

language = "English",

volume = "12",

pages = "2110--2117",

journal = "ChemPhysChem",

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T1 - Double-oxygen-atom transfer in reactions of CemO 2m+ (m=2-6) with C2H2

AU - Ding, Xun Lei

AU - Wu, Xiao Nan

AU - Zhao, Yan Xia

AU - Ma, Jia Bi

AU - He, Sheng Gui

PY - 2011/8/1

Y1 - 2011/8/1

N2 - Cerium oxide cluster cations (CemOn+, m=2-16; n=2m, 2m±1 and 2m±2) are prepared by laser ablation and reacted with acetylene (C2H2) in a fast-flow reactor. A time-of-flight mass spectrometer is used to detect the cluster distribution before and after the reactions. Reactions of stoichiometric CemO 2m+ (m=2-6) with C2H2 produce CemO2m-2+ clusters, which indicates a "double-oxygen-atom transfer" reaction CemO 2m++C2H2→CemO 2m-2++(CHO)2 (ethanedial). A single-oxygen-atom transfer reaction channel is also identified as CemO 2m++C2H2→CemO 2m-1++C2H2O (at least for m=2 and 3). Density functional theory calculations are performed to study reaction mechanisms of Ce2O4++C2H 2, and the calculated results confirm that both the single- and double-oxygen-atom transfer channels are thermodynamically and kinetically favourable.

AB - Cerium oxide cluster cations (CemOn+, m=2-16; n=2m, 2m±1 and 2m±2) are prepared by laser ablation and reacted with acetylene (C2H2) in a fast-flow reactor. A time-of-flight mass spectrometer is used to detect the cluster distribution before and after the reactions. Reactions of stoichiometric CemO 2m+ (m=2-6) with C2H2 produce CemO2m-2+ clusters, which indicates a "double-oxygen-atom transfer" reaction CemO 2m++C2H2→CemO 2m-2++(CHO)2 (ethanedial). A single-oxygen-atom transfer reaction channel is also identified as CemO 2m++C2H2→CemO 2m-1++C2H2O (at least for m=2 and 3). Density functional theory calculations are performed to study reaction mechanisms of Ce2O4++C2H 2, and the calculated results confirm that both the single- and double-oxygen-atom transfer channels are thermodynamically and kinetically favourable.

KW - cerium

KW - cluster compounds

KW - density functional calculations

KW - mass spectrometry

KW - reaction mechanisms

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DO - 10.1002/cphc.201100216

M3 - Article

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SN - 1439-4235

VL - 12

SP - 2110

EP - 2117

JO - ChemPhysChem

JF - ChemPhysChem

IS - 11

ER -

Double-oxygen-atom transfer in reactions of Ce_mO _2m⁺ (m=2-6) with C₂H₂

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