Oxidation of a butane fraction with hydrogen peroxide to oxygenates over a TPhPFe(III)OH/Al2O3 bioimitator
摘要
A mixture of aliphatic C1–C4 alcohols was obtained by hydroxylation of a mixture of hydrocarbon gases as a renewable raw material, which is the composition of the butane fraction (BF) (CH4—10.0%, C2H6—22.8%, C3H8—23.0%, i-C4H10—21.8%, n-C4H10—22.4%) obtained from the gas oil fraction at a local oil refinery. The hydroxylation process was carried out in a flow-through quartz reactor at atmospheric pressure and a temperature of 115–200 °C using hydrogen peroxide as a green oxidizer in the presence of a biomimetic catalyst iron tetraphenylporphyrin on aluminum oxide (TPhPFe(III)OH/Al2O3). The ratio of the obtained alcohols to each other depends on the process conditions: at 150 °C using a 30% aqueous solution of hydrogen peroxide, an oxygenate is obtained consisting of: CH2O—9.6%, CH3OH—44.7%, C2H5OH—12.3%, C3H7OH—14.5%, C4H9OH—15.1% and DME—3.8%, which can be used as an oxygenate additive to fuels to improve their qualities. The overall conversion of BF ranged from 86.4 to 95% depending on the process conditions. The mechanism of conversion of hydrocarbon gas into alcohols on the surface of a biomimetic catalyst is presented, which shows the combined action of the ligand (TPhPFe(III)OH) with the acid–base centers of the Al2O3 support.