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Alkylation of benzene with carbon dioxide to low-carbon aromatic hydrocarbons over bifunctional Zn-Ti/HZSM-5 catalyst
Frontiers of Chemical Science and Engineering ( IF 4.3 ) Pub Date : 2021-05-04 , DOI: 10.1007/s11705-021-2045-y
Xiangyu Liu , Yanling Pan , Peng Zhang , Yilin Wang , Guohao Xu , Zhaojie Su , Xuedong Zhu , Fan Yang

Alkylation of benzene to value-added, high octane number and low toxic toluene and xylenes provides a way to lower benzene content in gasoline pool, and is hence a method to promote fuel quality. On the other hand, CO2 accumulation in the atmosphere causes global warming and requires effective route for its valorization. Utilization of CO2 as a carbon source for benzene alkylation could achieve both goals. Herein, alkylation of benzene with CO2 and H2 was realized by a series of low-cost bifunctional catalysts containing zinc/titanium oxides (Zn/Ti oxides) and HZSM-5 molecular sieves in a fixed-bed reactor. By regulating and controlling oxygen vacancies of Zn/Ti oxides and the acidities of HZSM-5, benzene conversion and CO2 conversion reached 28.7% and 29.9% respectively, along with a total selectivity of toluene and xylene higher than 90%. In this process, more than 25% CO2 was effectively utilized and incorporated into the target products. Moreover, the mechanism of the reaction was analyzed and the course was simultaneously traced. CO2 was transformed into methanol firstly, and then methanol reacted with benzene generating toluene and xylene. The innovation provides a new method for upgrading of fuels and upcycling the emissions of CO2, which is of great environmental and economic benefits.



中文翻译:

双功能Zn-Ti / HZSM-5催化剂将苯与二氧化碳烷基化为低碳芳烃

苯烷基化为高附加值,高辛烷值和低毒的甲苯和二甲苯提供了降低汽油库中苯含量的方法,因此是提高燃油质量的一种方法。另一方面,CO 2在大气中的积累会导致全球变暖,并需要有效的途径来实现其增值。利用CO 2作为苯烷基化的碳源可以实现两个目标。在此,通过在固定床反应器中通过一系列包含锌/钛氧化物(Zn / Ti氧化物)和HZSM-5分子筛的低成本双功能催化剂实现了苯与CO 2和H 2的烷基化。通过调节和控制Zn / Ti氧化物的氧空位和HZSM-5的酸度,苯转化率和CO2的转化率分别达到28.7%和29.9%,并且甲苯和二甲苯的总选择性高于90%。在此过程中,有效利用了超过25%的CO 2并将其掺入目标产品中。此外,分析了反应机理并同时追踪了反应过程。首先将CO 2转化为甲醇,然后甲醇与苯反应生成甲苯和二甲苯。该创新提供了一种新的方法来升级燃料和提高CO 2排放的循环利用,这具有巨大的环境和经济效益。

更新日期:2021-05-05
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