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Direct CO2 hydrogenation to ethanol over supported Co2C catalysts: Studies on support effects and mechanism
Journal of Catalysis ( IF 6.5 ) Pub Date : 2019-12-27 , DOI: 10.1016/j.jcat.2019.11.038
Shunan Zhang , Xiaofang Liu , Zilong Shao , Hui Wang , Yuhan Sun

Direct CO2 hydrogenation to ethanol is one of the promising and emerging routes for the transformation of CO2 into value-added chemicals, but it remains a major challenge because of low ethanol selectivity and catalytic stability. In this work, Na-promoted cobalt catalysts supported on different materials (Al2O3, ZnO, AC, TiO2, SiO2, and Si3N4) were evaluated to elucidate the effects of supports. The SiO2- and Si3N4-supported catalysts exhibited efficient generation of ethanol with 18% CO2 conversion and 62% selectivity in the alcohol distribution at 250 °C, whereas CH4 was predominantly produced on other supported catalysts. Characterization results indicated that the Co2C active phase only remained intact on SiO2 and Si3N4 supports during reaction and exhibited excellent durability for 300 h, which was attributed to the existence of a strong metal–support interaction (SMSI) obtained by SiOCo bond formation. In situ DRIFTS results revealed that CO produced on Co2C inserted into CHx intermediates to form ethanol. Moreover, CO as the reactive intermediate could induce the regeneration and reconstruction of decomposed Co2C on the surface for catalytic sustainability.



中文翻译:

负载型Co 2 C催化剂上CO 2直接加氢制乙醇的负载效应及机理研究

将CO 2直接氢化为乙醇是将CO 2转化为增值化学品的有前途和新兴途径之一,但由于乙醇选择性低和催化稳定性低,它仍然是主要挑战。在这项工作中,评估了在不同材料(Al 2 O 3,ZnO,AC,TiO 2,SiO 2和Si 3 N 4)上负载的Na促进的钴催化剂,以阐明载体的作用。SiO 2和Si 3 N 4负载的催化剂显示出可有效生成含18%CO 2的乙醇在250°C时,乙醇分布具有较高的转化率和62%的选择性,而CH 4主要在其他负载型催化剂上产生。表征结果表明,在反应过程中,Co 2 C活性相仅在SiO 2和Si 3 N 4载体上完好无损,并且在300 h内表现出优异的耐久性,这归因于存在强金属-载体相互作用(SMSI)。 Si O Co键形成。原位DRIFTS结果表明,插入到CH x中的Co 2 C上产生的CO中间体形成乙醇。此外,CO作为反应性中间体可以诱导表面上分解的Co 2 C的再生和重建,从而实现催化的可持续性。

更新日期:2019-12-29
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