期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 17, 期 17, 页码 11277-11283出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c5cp00726g
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资金
- European Regional Development Fund Franco-British INTERREG IVA [E3C3, 4274]
This work is a mechanistic study of total and partial methanol photooxidation using operando FTIR coupled to gas phase analysis techniques (gas-IR and MS). Methoxy and formate/formyl species play a key role in the reaction. Methoxy species are formed by thermal and photochemical dissociation of methanol. The formation of methylformate is favored by a high surface coverage by methoxy species. Surface and/or bridged oxygen atoms are also important actors. Steady State Isotopic Transient Kinetic Analysis (SSITKA) experiments showed that the limiting step is the conversion of chemisorbed formyl/formate and that methylformate is a secondary product from a reaction between methoxy and neighboring formyl species. Methanol concentration, among other reaction parameters, influences greatly the selectivity of photooxidation.
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