H2 dissociation by Au1-doped closed-shell titanium oxide cluster anions

Li Xue Jiang; Xiao Na Li; Zi Yu Li; Hai Fang Li; Sheng Gui He

doi:10.1063/1674-0068/31/cjcp1805107

H₂ dissociation by Au₁-doped closed-shell titanium oxide cluster anions

Li Xue Jiang, Xiao Na Li^*, Zi Yu Li, Hai Fang Li, Sheng Gui He

^*Corresponding author for this work

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

6 Citations (Scopus)

Abstract

Dissociation of molecular hydrogen (H₂) is extensively studied to understand the mechanism of hydrogenation reactions. In this study, H₂ dissociation by Au1-doped closed-shell titanium oxide cluster anions AuTi₃O₇^- and AuTi₃O₈^- has been identified by mass spectrometry and quantum chemistry calculations. The clusters were generated by laser ablation and mass-selected to react with H₂ in an ion trap reactor. In the reaction of AuTi₃O₈^- with H₂, the ion pair Au⁺-O₂^2- rather than Au⁺-O^2- is the active site to promote H₂ dissociation. This finding is in contrast with the previous result that the lattice oxygen is usually the reactive oxygen species in H₂ dissociation. The higher reactivity of the peroxide species is further supported by frontier molecular orbital analysis. This study provides new insights into gold catalysis involving H₂ activation and dissociation.

Original language	English
Pages (from-to)	457-462
Number of pages	6
Journal	Chinese Journal of Chemical Physics
Volume	31
Issue number	4
DOIs	https://doi.org/10.1063/1674-0068/31/cjcp1805107
Publication status	Published - 1 Aug 2018
Externally published	Yes

Keywords

Closed-shell anions
Density functional theory calculations
Gold
H dissociation
Mass spectrometry

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10.1063/1674-0068/31/cjcp1805107

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title = "H2 dissociation by Au1-doped closed-shell titanium oxide cluster anions",

abstract = "Dissociation of molecular hydrogen (H2) is extensively studied to understand the mechanism of hydrogenation reactions. In this study, H2 dissociation by Au1-doped closed-shell titanium oxide cluster anions AuTi3O7- and AuTi3O8- has been identified by mass spectrometry and quantum chemistry calculations. The clusters were generated by laser ablation and mass-selected to react with H2 in an ion trap reactor. In the reaction of AuTi3O8- with H2, the ion pair Au+-O22- rather than Au+-O2- is the active site to promote H2 dissociation. This finding is in contrast with the previous result that the lattice oxygen is usually the reactive oxygen species in H2 dissociation. The higher reactivity of the peroxide species is further supported by frontier molecular orbital analysis. This study provides new insights into gold catalysis involving H2 activation and dissociation.",

keywords = "Closed-shell anions, Density functional theory calculations, Gold, H dissociation, Mass spectrometry",

author = "Jiang, \{Li Xue\} and Li, \{Xiao Na\} and Li, \{Zi Yu\} and Li, \{Hai Fang\} and He, \{Sheng Gui\}",

note = "Publisher Copyright: {\textcopyright} 2018 Chinese Physical Society.",

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doi = "10.1063/1674-0068/31/cjcp1805107",

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T1 - H2 dissociation by Au1-doped closed-shell titanium oxide cluster anions

AU - Jiang, Li Xue

AU - Li, Xiao Na

AU - Li, Zi Yu

AU - Li, Hai Fang

AU - He, Sheng Gui

PY - 2018/8/1

Y1 - 2018/8/1

N2 - Dissociation of molecular hydrogen (H2) is extensively studied to understand the mechanism of hydrogenation reactions. In this study, H2 dissociation by Au1-doped closed-shell titanium oxide cluster anions AuTi3O7- and AuTi3O8- has been identified by mass spectrometry and quantum chemistry calculations. The clusters were generated by laser ablation and mass-selected to react with H2 in an ion trap reactor. In the reaction of AuTi3O8- with H2, the ion pair Au+-O22- rather than Au+-O2- is the active site to promote H2 dissociation. This finding is in contrast with the previous result that the lattice oxygen is usually the reactive oxygen species in H2 dissociation. The higher reactivity of the peroxide species is further supported by frontier molecular orbital analysis. This study provides new insights into gold catalysis involving H2 activation and dissociation.

AB - Dissociation of molecular hydrogen (H2) is extensively studied to understand the mechanism of hydrogenation reactions. In this study, H2 dissociation by Au1-doped closed-shell titanium oxide cluster anions AuTi3O7- and AuTi3O8- has been identified by mass spectrometry and quantum chemistry calculations. The clusters were generated by laser ablation and mass-selected to react with H2 in an ion trap reactor. In the reaction of AuTi3O8- with H2, the ion pair Au+-O22- rather than Au+-O2- is the active site to promote H2 dissociation. This finding is in contrast with the previous result that the lattice oxygen is usually the reactive oxygen species in H2 dissociation. The higher reactivity of the peroxide species is further supported by frontier molecular orbital analysis. This study provides new insights into gold catalysis involving H2 activation and dissociation.

KW - Closed-shell anions

KW - Density functional theory calculations

KW - Gold

KW - H dissociation

KW - Mass spectrometry

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DO - 10.1063/1674-0068/31/cjcp1805107

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VL - 31

SP - 457

EP - 462

JO - Chinese Journal of Chemical Physics

JF - Chinese Journal of Chemical Physics

IS - 4

ER -

H₂ dissociation by Au₁-doped closed-shell titanium oxide cluster anions

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Keywords

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