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Thermal Methane Conversion to Formaldehyde Promoted by Single Platinum Atoms in PtAl 2 O 4 − Cluster Anions
Author(s) -
Zhao YanXia,
Li ZiYu,
Yuan Zhen,
Li XiaoNa,
He ShengGui
Publication year - 2014
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201403953
Subject(s) - chemistry , methane , platinum , oxide , inorganic chemistry , formaldehyde , iridium , density functional theory , cluster (spacecraft) , photochemistry , computational chemistry , catalysis , organic chemistry , computer science , programming language
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 − 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 − 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.