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Catalytic wet peroxide oxidation of phenol on Fe-ZSM-5/PSSF membrane catalysts: Effect of framework Fe by hydrothermal synthesis

机译:Fe-ZSM-5 / PSSF膜催化剂上苯酚的催化湿过氧化物氧化:水热合成框架Fe的影响

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Two kinds of zeolite membrane catalysts, Fe-ZSM-5/PSSF and Fe2O3/ZSM-5/PSSF, were synthesized by hydrothermal method and incipient wetness impregnation method respectively, and tested for catalytic wet peroxide oxidation (CWPO) of phenol in the fixed bed reactor. The paper-like stainless steel fiber (PSSF) were prepared by a combined papermaking and sintering process. Then hydrothermal and impregnation methods were applied to coat Fe-ZSM-5 as well as Fe2O3/ZSM-5 membrane catalyst on PSSF respectively. Framework Fe3+ species on the Fe-ZSM-5/PSSF zeolite membrane catalysts were characterized and tested for phenol oxidation in the fixed bed reactor. In addition, the effects of Si/Fe, temperature and residence time on catalyst performance were investigated. Results showed that Fe-ZSM-5/PSSF with Si/Fe = 120 showed highest activity. Higher temperature and longer residence time can improve the catalytic performance and the existence of the framework Fe3+ species over Fe-ZSM-5/PSSF can enhance the catalytic efficiency of phenol, with phenol conversion of over 99.0% and TOC conversion of 55.6% under condition of 4 cm bed height, 2 mL/min feed flow rate and 80 degrees C. Catalytic activity of Fe-ZSM-5/PSSF was dramatically increased compared to the Fe2O3/ZSM-5/PSSF, indicating the key role of framework Fe3+ played in the CWPO process. Finally, the stability test results showed that a relatively low decrease in activity of Fe-ZSM-5/PSSF (Si/Fe = 120) can be found after three consecutive runs (21 h).
机译:通过水热法和初始湿润浸渍法合成两种沸石膜催化剂,Fe-ZSM-5 / PSSF和Fe 2 O 3 / ZSM-5 / PSSF,并测试固定的苯酚的催化湿过氧化物氧化(CWPO)床反应器。纸状不锈钢纤维(PSSF)通过组合的造纸和烧结过程制备。然后将水热和浸渍方法分别涂覆Fe-ZSM-5以及PSSF上的Fe 2 O 3 / ZSM-5膜催化剂。 Fe-ZSM-5 / PSSF沸石膜催化剂上的框架Fe3 +物种的特征和测试用于固定床反应器中的苯酚氧化。此外,研究了Si / Fe,温度和停留时间对催化剂性能的影响。结果表明,具有Si / Fe = 120的Fe-ZSM-5 / PSSF显示出最高的活性。较高的温度和较长的停留时间可以改善催化性能,并且Fe-ZSM-5 / PSSF上的框架Fe3 +物种的存在可以增强苯酚的催化效率,苯酚转化超过99.0%和TOC转化率为55.6%的病症与Fe2O3 / ZSM-5 / PSSF相比,4厘米床高度,2mL / min进料流速和80℃的催化活性大致增加了Fe-ZSM-5 / PSSF的催化活性,表明框架Fe3 +发挥的关键作用在CWPO过程中。最后,稳定性测试结果表明,在连续三次运行后,可以发现Fe-ZSM-5 / PSSF(Si / Fe = 120)的活性相对低的减少(21小时)。

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