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Properties and catalytic performance in phenol hydroxylation of iron on zeolite beta prepared by different methods

机译:不同方法制备的β型沸石上铁的酚羟基化性质及催化性能

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Iron (Fe) was loaded on zeolite beta (BEA) in ammonium (NH(4)BEA) or proton (HBEA) forms by various methods. Fe/HBEA-LSIE and Fe/NH(4)BEA-LSIE were prepared by liquid state ion exchange (LSIE). This method resulted in low Fe loading and a good dispersion. The form of Fe was Fe2O3 mainly located at the ion exchange position in the zeolite channels. Fe/HBEA-IWI and Fe/HBEA-PM were prepared by incipient wetness impregnation (IWI) and physical mixing (PM), respectively. Both catalysts had higher Fe loading and larger Fe2O3 particles located on both external surface and in the zeolite channels. Despite the different loadings, all samples gave similar phenol conversion in phenol hydroxylation, around 60 % and yielded products catechol (CAT) and hydroquinone (HQ) with the CAT/HQ mole ratio 2:1. After the catalytic testing, all catalysts had a dark color from coking. A further investigation revealed a formation of coke and organic acids. According to temperature programmed oxidation (TPO), heavy coke was produced from Fe/HBEA-LSIE and Fe/NH(4)BEA-LSIE. The coke from Fe/HBEA-LSIE was heavier than that from Fe/NH(4)BEA-LSIE. Only light coke was produced from Fe/HBEA-IWI and Fe/HBEA-PM.
机译:通过各种方法将铁(Fe)负载在铵(NH(4)BEA)或质子(HBEA)形式的沸石β(BEA)上。 Fe / HBEA-LSIE和Fe / NH(4)BEA-LSIE通过液相离子交换(LSIE)制备。该方法导致低的铁负载量和良好的分散性。 Fe的形式为Fe 2 O 3,主要位于沸石通道中的离子交换位置。 Fe / HBEA-IWI和Fe / HBEA-PM分别通过初期湿润浸渍(IWI)和物理混合(PM)制备。两种催化剂在外表面和沸石通道中均具有较高的Fe负载量和较大的Fe 2 O 3颗粒。尽管加载量不同,但所有样品在酚羟基化中的苯酚转化率均相似,约为60%,并产生了CAT / HQ摩尔比为2:1的邻苯二酚(CAT)和对苯二酚(HQ)。催化测试后,所有催化剂的焦化颜色均为深色。进一步的调查表明形成了焦炭和有机酸。根据程序升温氧化(TPO),Fe / HBEA-LSIE和Fe / NH(4)BEA-LSIE生产了重焦炭。 Fe / HBEA-LSIE的焦炭比Fe / NH(4)BEA-LSIE的焦炭重。 Fe / HBEA-IWI和Fe / HBEA-PM仅产生轻质焦炭。

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