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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Redox Chemistry of Gaseous Reactants Inside Photoexcited FeAlPO_4 Molecular Sieve
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Redox Chemistry of Gaseous Reactants Inside Photoexcited FeAlPO_4 Molecular Sieve

机译：FeAlPO_4分子筛内气态反应物的氧化还原化学

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摘要

The reactivity of ligand-to-metal charge transfer excited Fe centers of FeAlPO_4-5 molecular sieve at the gas-micropore interface has been probed by in situ FT-IR spectroscopy. Laser light in the region 350-430 nm was used to excite the metal centers, and reaction was induced between methanol or 2-propanol and O_2. Acetone and H_2O are the observed products of the 2-propanol + O_2 system, while the reaction of methanol with O_2 yields formic acid, methyl formate, and H_2O as final products. These originate from secondary thermal reaction of initially produced formaldehyde and hydrogen peroxide. The primary step of the proposed mechanism involves one-electron reduction of O_2 by transient Fe~(+II) under concurrent donation of an electron to the hole of framework oxygen by the alcohol molecule. The efficient reaction suggests that the photoreduced Fe center of the molecular sieve has a substantially stronger reducing power than the conduction band electrons of dense-phase Fe_2O_3 semiconductor particles.
机译：通过原位FT-IR光谱探测了FeAlPO_4-5分子筛在气体-微孔界面处的配体到金属的电荷转移激发的Fe中心的反应性。使用350-430 nm区域的激光激发金属中心，并在甲醇或2-丙醇与O_2之间引发反应。丙酮和H_2O是2-丙醇+ O_2系统的产物，而甲醇与O_2的反应则生成甲酸，甲酸甲酯和H_2O作为最终产物。这些源自最初产生的甲醛和过氧化氢的二次热反应。拟议机制的第一步涉及在醇分子同时向骨架氧的空穴提供电子的同时，由瞬态Fe〜（+ II）单电子还原O_2。有效反应表明，分子筛的光还原Fe中心具有比浓相Fe_2O_3半导体颗粒的导带电子明显更强的还原能力。

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