铁钾基复合氧化物上CO_(2)氧化乙苯脱氢制苯乙烯的原位DRIFTS研究  

In situ DRIFTS investigation of ethylbenzene oxidative dehydrogenation for styrene with CO_(2)over Fe-K mixed oxide catalysts

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作  者:曾铁强 查凯文 王晨宇 张征湃 宋磊 缪长喜 ZENG Tieqiang;ZHA Kaiwen;WANG Chenyu;ZHANG Zhengpai;SONG Lei;MIAO Changxi(Sinopec(Shanghai)Research Institute of Petrochemical Technology Co.,Ltd.,Shanghai 201208,China)

机构地区:[1]中石化(上海)石油化工研究院有限公司,上海201208

出  处:《石油化工》2024年第12期1704-1711,共8页Petrochemical Technology

摘  要:采用湿法造粒法制备了Fe-K,Fe-K-Ce,Fe-K-Ce-Mo复合氧化物催化剂,利用原位漫反射傅里叶变换红外光谱技术考察了催化剂在CO_(2)氧化乙苯脱氢制苯乙烯反应中的反应机理、促进作用和构效关系。实验结果表明,在CO_(2)氧化乙苯脱氢反应中,Ce的加入提高了催化剂的活性,Mo改性提升了苯乙烯的选择性。催化剂经改性后促进了碳酸盐物种的形成,Fe-K-Ce催化剂形成了更多桥联碳酸盐物种,Fe-K-Ce-Mo催化剂增加了双齿碳酸盐物种。这些碳酸盐物种在高温下分解进行CO_(2)脱附并释放活性位点,乙苯会吸附在这些位点上脱氢生成苯乙烯和H2,H2与CO_(2)进行逆水煤气变换反应。此外,引入CO_(2)后缩短了催化剂的活化诱导期,提高了苯乙烯产量。The composite oxide catalysts Fe-K,Fe-K-Ce and Fe-K-Ce-Mo were prepared by the wet granulation method.In situ diffuse reflectance infrared Fourier transform spectroscopy were performed to investigate the reaction mechanism,promotional effects and structure-activity relationship of catalysts in ethylbenzene oxidative dehydrogenation to styrene reactions in the presence of CO_(2).The experimental results show that the Ce addition improved catalytic activity for Fe-K catalysts,and the Mo modification increased styrene selectivity.The modified catalysts promoted carbonate species formation,Fe-K-Ce and Fe-K-Ce-Mo catalysts formed more bridged and bidentate carbonate species respectively.These carbonate species would decompose and desorb CO_(2),and release active sites under high temperature,then ethylbenzene would be adsorbed on these sites and dehydrogenate to generate styrene and H2,and then H2 was available to react with CO_(2)from carbonate species or gas phase CO_(2)via the reverse water gas reaction.Furthermore,after CO_(2)introduction,the activation induction periods of all catalysts were shortened and styrene production was improved.

关 键 词:乙苯 脱氢 苯乙烯 二氧化碳 原位漫反射傅里叶变换红外光谱 

分 类 号:TQ241.2[化学工程—有机化工]

 

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