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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Mechanistic Study of CH_3OH + O_2 Photoredox Reaction in FeAlPO_4 Sieve by Time-Resolved FT-IR Spectroscopy
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Mechanistic Study of CH_3OH + O_2 Photoredox Reaction in FeAlPO_4 Sieve by Time-Resolved FT-IR Spectroscopy

机译：时间分辨FT-IR光谱法研究FeAlPO_4筛中CH_3OH + O_2光氧化还原反应的机理

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摘要

The mechanism of the ligand-to-metal charge transfer (LMCT) induced reaction of methanol and O_2 at the gas-micropore interface of a FeAlPO_4-5 sieve has been studied by time-resolved FT-IR spectroscopy. Measurements using the rapid-scan method revealed that the final products, HCO_2~-…Fe and H_2O, emerge with a rise time of 4 s (250 K) by decomposition of the two-electron-transfer intermediate, HO_2CH_2OH. Intermediacy of hydroxymethylhydroperoxide was established by direct detection by step-scan FT-IR spectroscopy on the 500 microsecond time scale and by monitoring of its photodissociation products HCO_2H + H_2O on the millisecond and second time scale. Formaldehyde was observed as minor two-electron oxidation product. The fast rise of the HO_2CH_2OH intermediate strongly suggests that it is formed by direct coupling of HOO and CH_2OH radicals. This constitutes the most conclusive evidence yet for the formation of a hydroperoxy radical and hydroxymethyl radical as the primary one-electron-transfer products of the reaction of CH_3OH and O_2 at LMCT-excited framework Fe centers.
机译：通过时间分辨FT-IR光谱研究了配体-金属电荷转移（LMCT）诱导的甲醇和O_2在FeAlPO_4-5分子筛的气-微孔界面反应的机理。使用快速扫描法进行的测量表明，最终产物HCO_2〜-…Fe和H_2O通过双电子转移中间体HO_2CH_2OH的分解以4 s（250 K）的上升时间出现。羟甲基氢过氧化物的中间体是通过在500微秒的时间尺度上通过步进扫描FT-IR光谱法直接检测并在毫秒和第二时间尺度上通过监测其光解产物HCO_2H + H_2O来建立的。甲醛被认为是次要的两电子氧化产物。 HO_2CH_2OH中间体的快速升高强烈表明它是由HOO和CH_2OH自由基的直接偶联形成的。这构成了迄今为止最确凿的证据，证明氢过氧自由基和羟甲基自由基是LMCT激发的骨架Fe中心CH_3OH和O_2反应的主要单电子转移产物。

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