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On the enhanced sulfur and coking tolerance of Ni-Co-rare earth oxide catalysts for the dry reforming of methane
Journal of Catalysis ( IF 7.3 ) Pub Date : 2020-12-03 , DOI: 10.1016/j.jcat.2020.11.028
Changyi Jiang , Emily Loisel , David A. Cullen , James A. Dorman , Kerry M. Dooley

Sulfur and coking tolerance of Ni-based dry reforming catalysts were examined. Catalysts utilizing both Ce/Zr and Ce/La oxide supports, some with additional Co, were tested. Long-term reaction runs were conducted with and without sulfur in the feed. Catalysts were also characterized by STEM, XPS, XAFS and XANES and CO chemisorption. Only catalysts where Co was also present, and supported on the Ce-Zr oxide, were capable of extended sulfur tolerance at >20 ppm sulfur. This tolerance, along with a greatly reduced coking rate, is linked to Co in intimate contact with Ni, the mixture existing as clusters anchored and influenced electronically by the oxide support. The activation of methane takes place on these sites. Larger metal aggregates formed by ripening during reaction appear to be spectators. The measured activation energies for dry reforming suggest that CO2 activation takes place at the oxide interface, and is a kinetically significant step.



中文翻译:

甲烷干重整制镍钴稀土氧化物催化剂的硫和焦化耐受性提高

研究了镍基干重整催化剂的硫和焦化耐受性。测试了同时使用Ce / Zr和Ce / La氧化物载体(其中一些还带有Co)的催化剂。进料中有无硫的情况下进行了长期反应。催化剂还通过STEM,XPS,XAFS和XANES以及CO化学吸附进行表征。只有同时还存在Co并负载在Ce-Zr氧化物上的催化剂才能在> 20 ppm硫的条件下扩展耐硫性。这种耐受性以及大大降低的焦化率与Co与Ni紧密接触有关,Co以Ni团簇形式存在,混合物被氧化物载体锚定并受到电子影响。甲烷的活化发生在这些位置。通过在反应过程中成熟而形成的较大的金属聚集体似乎是观众。2活化发生在氧化物界面,是一个重要的动力学步骤。

更新日期:2020-12-23
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