Journal of Environmental Chemical Engineering ( IF 7.4 ) Pub Date : 2022-09-16 , DOI: 10.1016/j.jece.2022.108609 Zhiying Liu , Xiaohui Sun , Yulin Li , Zhuyin Sui , Xiufeng Xu
The ordered mesoporous Al2O3 material was employed as support to prepare the CeO2-Co3O4 binary oxide catalysts for N2O-assisted oxidative dehydrogenation of ethylbenzene (EB), which was treated both as an effective method of styrene (ST) production and a high value-added utilization of the greenhouse gas. The catalytic performance was observed for the optimal 0.3Ce-7Co/OMA catalyst, which achieved 52.1% EB conversion with 88.7% selectivity toward ST at temperature as low as 500 ºC, far exceeding any other reported catalyst systems. Characterization results showed that an increase in the Co content led to a partial destruction of the order degree of pores, but maintained the mesoporous structure. The Ce modification not only decreased the particle size (<12 nm), considerably boosting the specific surface area, but also weakened the Co-O bond, making more O species available for the EB conversion. Studies on the carbon deposition formed during the catalytic runs revealed that the carbon deposited at the initial stage of reaction acted directly as the catalytically active sites enhanced the EB conversion. As the reaction progressed, the dynamic equilibrium between carbon deposition and burning relieved the loss of active sites and maintained the stability of catalyst activity. In addition, the excellent regeneration property of 0.3Ce-7Co/OMA catalyst indicated that N2O, which was used as an oxidizing agent, protected the catalyst against the formation of inactive carbonaceous deposition.
中文翻译:
有序介孔Al2O3上沉积的Ce-Co物种和焦炭在N2O辅助乙苯氧化脱氢中的催化作用研究
以有序介孔Al 2 O 3材料为载体制备CeO 2 -Co 3 O 4二元氧化物催化剂用于N 2乙苯(EB)的O辅助氧化脱氢,既被视为生产苯乙烯(ST)的有效方法,又被视为温室气体的高附加值利用方法。观察到最佳的 0.3Ce-7Co/OMA 催化剂的催化性能,该催化剂在低至 500 ºC 的温度下实现了 52.1% 的 EB 转化率和 88.7% 的 ST 选择性,远远超过任何其他报道的催化剂体系。表征结果表明,Co含量的增加导致孔隙有序度的部分破坏,但保持了介孔结构。Ce 改性不仅减小了粒径(<12 nm),显着提高了比表面积,而且削弱了 Co-O 键,使更多的 O 物种可用于 EB 转化。对催化运行过程中形成的碳沉积的研究表明,在反应初始阶段沉积的碳直接作为催化活性位点提高了 EB 的转化率。随着反应的进行,碳沉积和燃烧之间的动态平衡缓解了活性位点的损失,保持了催化剂活性的稳定性。此外,0.3Ce-7Co/OMA催化剂优异的再生性能表明N用作氧化剂的2 O 保护催化剂免受惰性碳质沉积物的形成。