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Ethyl benzene oxidative dehydrogenation to styrene on Al-B and Al-B-Sb catalysts
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2017-12-28 , DOI: 10.1016/j.apcata.2017.12.023
Abdulrahim A. Al-Zahrani , Nagaraju Pasupulety , Muhammad A. Daous , Hafedh Driss , Arshid M. Ali , Sharif F. Zaman , Lachezar A. Petrov

Alumina (Al), alumina-boron (Al-15B), alumina-boron-antimony (Al-B-Sb) and alumina-antimony (Al-15Sb) catalysts were synthesized by sol-gel method using ethanol as a solvent and ammonia gas as a gel forming agent. These catalysts were studied for the dehydrogenation of ethylbenzene (EB) to styrene in the presence of oxygen and steam. The reaction was carried out in the temperature range of 450-500 °C with EB contact time 0.54 gcat.s/cm3. The synthesized catalysts were characterized by using N2-physisorption, XRD, XPS, TEM-HRTEM-EDS and NH3-TPD-mass spectral analysis techniques. At 475 °C, only 58% of styrene selectivity with 32% of EB conversion was observed on Al. Addition of 15 mol.% of B to Al significantly enhanced the selectivity of styrene to 94% with 46% EB conversion at 475 °C. Addition of 15 mol.% Sb to Al reduced the EB conversion (38%) and styrene selectivity (75%) compared to Al-15B catalyst. Interestingly, small amount of Sb (5 mol.%) addition to Al-B improved the EB conversion to 52.5% with 92% of styrene selectivity at 475 °C. The acid sites of weak and moderate strength were increased in Al-15B catalyst compared to Al. Boron played a dual role as Al densification suppressing agent and to some extent deposited on the surface of Al which improved the styrene selectivity. However, small amount of Sb addition to Al-15B not only retained weak and moderate strength acid sites of Al-B but also generated acid sites of Sb which led to the formation of N2O and NO during NH3-TPD-mass analysis. Hence, the styrene yield (48.8%) was improved on Al-B-5Sb compared to Al-15B catalyst (43%). It is noteworthy that Al-15B and Al-B-5Sb catalysts were stable for more than 60h of reaction.



中文翻译:

Al-B和Al-B-Sb催化剂上乙苯氧化脱氢制苯乙烯

以乙醇为溶剂,氨水为溶胶-凝胶法合成了氧化铝(Al),氧化铝-硼(Al-15B),氧化铝-硼-锑(Al-B-Sb)和氧化铝-锑(Al-15Sb)催化剂。气体作为凝胶形成剂。研究了这些催化剂在氧气和蒸汽存在下将乙苯(EB)脱氢成苯乙烯的方法。将反应物的温度范围内的450-500进行℃用EB接触时间0.54克.S /厘米3。利用N 2-物理吸附,XRD,XPS,TEM-HRTEM-EDS和NH 3对催化剂进行了表征。-TPD-质谱分析技术。在475°C下,在Al上仅观察到58%的苯乙烯选择性和32%的EB转化率。在475°C下,EB转化率为46%,向Al中添加15 mol。%的B可以显着提高苯乙烯的选择性,达到94%。与Al-15B催化剂相比,向Al中添加15mol。%的Sb降低了EB转化率(38%)和苯乙烯选择性(75%)。有趣的是,在475°C下,向Al-B中添加少量Sb(5 mol。%)可使EB转化率提高至52.5%,苯乙烯选择性达到92%。与Al相比,Al-15B催化剂中弱和中等强度的酸位增加了。硼起着铝致密化剂的双重作用,并在一定程度上沉积在铝的表面上,从而提高了苯乙烯的选择性。然而,NH 3 -TPD质量分析过程中的2 O和NO 。因此,与Al-15B催化剂(43%)相比,在Al-B-5Sb上苯乙烯的产率(48.8%)提高了。值得注意的是,Al-15B和Al-B-5Sb催化剂在60小时以上的反应中均保持稳定。

更新日期:2017-12-28
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