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Syngas production by methane tri-reforming: Effect of Ni/CeO2 synthesis method on oxygen vacancies and coke formation
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2021-12-18 , DOI: 10.1016/j.jcou.2021.101853
Chayene Gonçalves Anchieta 1 , Elisabete Moreira Assaf 2 , José Mansur Assaf 1
Affiliation  

The CH4 tri-reforming process can contribute to mitigating CO2 emissions and enables the formation of syngas with different H2/CO ratios. Ni catalysts supported on CeO2 were synthesized by hydrothermal and ionothermal methods and were applied in methane tri-reforming reactions with GHSV of 48,000 mL/g.h, at atmospheric pressure and temperature of 800 °C. The catalytic activity in the tri-reforming reaction was enhanced by changing the morphological properties of the catalyst by appropriate selection of the amount of ionic liquid used in the synthesis procedure. Changing the composition resulted in methane conversion increasing from 60 % to 95 % and carbon dioxide conversion increasing from 40 % to 55 %. Increased Ni dispersion was related to the oxygen vacancies on the Ni-Ce surface, which created interfacial active sites. The results of XANES combined with XPS revealed that a partial reduction of Ni species contributed to high hydrogen yields, due to the distribution of active sites over the catalyst surface. These sites remained active during 5 h, demonstrating the positive effect of the ionic liquid used in the CeO2 synthesis. In addition, post-reaction characterization results showed Ni re-oxidation on the ceria support produced without ionic liquid.



中文翻译:

甲烷三重重整制合成气:Ni/CeO2合成方法对氧空位和焦炭形成的影响

CH 4三重重整工艺有助于减少CO 2排放并能够形成具有不同H 2 /CO 比率的合成气。负载在 CeO 2上的 Ni 催化剂分别采用水热法和离子热法合成,并应用于甲烷三重重整反应,GHSV为48,000 mL / gh,常压和温度为800°C。The catalytic activity in the tri-reforming reaction was enhanced by changing the morphological properties of the catalyst by appropriate selection of the amount of ionic liquid used in the synthesis procedure. 改变组成导致甲烷转化率从 60% 增加到 95%,二氧化碳转化率从 40% 增加到 55%。Ni 分散的增加与 Ni-Ce 表面上的氧空位有关,这产生了界面活性位点。XANES 与 XPS 结合的结果表明,由于活性位点分布在催化剂表面,Ni 物质的部分还原有助于高产氢率。2合成。此外,反应后表征结果表明镍在没有离子液体的情况下生产的二氧化铈载体上发生了再氧化。

更新日期:2021-12-18
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