Thermal C-O coupling reactions of Ta methylene clusters [TaCH] ( = 1, 4) with O
Cationic tantalum carbenes [TaCH 2 ] + and [Ta 4 CH 2 ] + , products of thermal methane dehydrogenation, are collected and stored in a ring-electrode ion trap. In there, potential C-O coupling reactions are probed by exposing the tantalum carbenes to dioxygen in the presence of helium buffer gas, th...
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| Published in | Physical chemistry chemical physics : PCCP Vol. 21; no. 37; pp. 2743 - 2749 |
|---|---|
| Main Authors | , , , , |
| Format | Journal Article |
| Published |
25.09.2019
|
| Online Access | Get full text |
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| Summary: | Cationic tantalum carbenes [TaCH
2
]
+
and [Ta
4
CH
2
]
+
, products of thermal methane dehydrogenation, are collected and stored in a ring-electrode ion trap. In there, potential C-O coupling reactions are probed by exposing the tantalum carbenes to dioxygen in the presence of helium buffer gas, thereby facilitating reactions under-well defined multi-collision conditions at 300 K. Time-of-flight mass spectrometry determines the time-dependent reaction products and a kinetic analysis illustrates significantly different selectivities. The cationic tantalum atom and tetramer systems undergo coupling reactions, which may lead to the formation of value-added products from the oxidation of methane. In particular, the reaction of [Ta
4
CH
2
]
+
with oxygen demonstrates an increased selectivity towards the formation of a formaldehyde equivalent.
Cationic tantalum carbenes [TaCH
2
]
+
and [Ta
4
CH
2
]
+
, products of methane dehydrogenation, are reacted with dioxygen in an ion trap. Detected products suggest a formation of value-added molecules originating from C-O coupling reactions. |
|---|---|
| Bibliography: | 10.1039/c9cp02739d Electronic supplementary information (ESI) available: Additional mass spectra under different condition for the confirmation of species assignment and the description of rate coefficients, errors and collision rates, together with the comparison of bare tantalum species and corresponding carbenes in the reaction with methane. See DOI |
| ISSN: | 1463-9076 1463-9084 |
| DOI: | 10.1039/c9cp02739d |