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Strong activity-based volcano-type relationship for dry reforming of methane through modulating Ni-CeO2 interaction over Ni/CeO2-SiO2 catalysts
Chem Catalysis ( IF 11.5 ) Pub Date : 2024-11-21 , DOI: 10.1016/j.checat.2024.101189
Yufeng Li, Zhenwei Li, Nan Wang, Yajun Zha, Ke Zheng, Yuebing Xu, Bing Liu, Xiaohao Liu

The dry reforming of methane (DRM) reaction holds significance for efficient conversion of CH4 and CO2 into syngas for the subsequent production of premium fuels and high-value chemicals. However, catalyst deactivation is easily caused by carbon deposition over Ni-based catalysts. Here, we investigated the effects of ultrasmall CeO2 nano-islands on the DRM reaction and found a strong volcano-type relationship between CeO2 content and reaction activity over Ni/CeO2-SiO2 catalysts. A suitable CeO2 amount can only slightly suppress CH4 dissociation but largely promote carbon species elimination. More importantly, the presence of these CeO2 nano-islands positively affected the types and location of coke species by “carbon-phobic effect” and thus alleviated coverage of Ni active sites. As a result, a higher TOFCH4 was obtained by an increase of about 82% and a continuous 2,000-h run almost without any side reaction, and deactivation was achieved along with CO2 and CH4 conversions at about 96% and 92%, respectively.

中文翻译:


通过调节 Ni/CeO2-SiO2 催化剂上的 Ni-CeO2 相互作用对甲烷进行干重整的强活性火山型关系



甲烷干重整 (DRM) 反应对于将 CH4 和 CO2 有效转化为合成气,用于随后生产优质燃料和高价值化学品具有重要意义。然而,催化剂失活很容易由镍基催化剂上的碳沉积引起。在这里,我们研究了超小 CeO2 纳米岛对 DRM 反应的影响,发现 CeO2 含量与 Ni/CeO2-SiO 2 催化剂的反应活性之间存在很强的火山型关系。适量的 CeO2 只能略微抑制 CH4 解离,但在很大程度上促进碳物质的消除。更重要的是,这些 CeO2 纳米岛的存在通过“疏碳效应”对焦炭种类的类型和位置产生了积极影响,从而减轻了 Ni 活性位点的覆盖率。结果,通过增加约 82% 和连续运行 2,000 小时,几乎没有任何副反应,获得了更高的 TOFCH4,并且分别以约 96% 和 92% 的 CO2 和 CH4 转化率实现了失活。
更新日期:2024-11-21
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