通过调节 Ni/CeO2-SiO2 催化剂上 Ni-CeO2 的相互作用实现甲烷干转化的强活性火山型关系

IF 11.5 Q1 CHEMISTRY, PHYSICAL Chem Catalysis 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
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引用次数: 0

摘要

甲烷干重整(DRM)反应对于将甲烷(CH4)和二氧化碳(CO2)高效转化为合成气,进而生产优质燃料和高价值化学品具有重要意义。然而,镍基催化剂上的碳沉积很容易导致催化剂失活。在此,我们研究了超小型纳米 CeO2 对 DRM 反应的影响,发现在 Ni/CeO2-SiO2 催化剂上,CeO2 含量与反应活性之间存在着强烈的火山型关系。合适的 CeO2 含量只能轻微抑制 CH4 的解离,却能在很大程度上促进碳物种的消除。更重要的是,纳米 CeO2 的存在通过 "疏碳效应 "对焦炭物种的类型和位置产生了积极影响,从而减轻了对 Ni 活性位点的覆盖。结果,TOFCH4 提高了约 82%,连续运行 2,000 小时几乎没有发生任何副反应,在实现去活化的同时,二氧化碳和甲烷的转化率分别达到约 96% 和 92%。
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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
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.
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来源期刊
CiteScore
10.50
自引率
6.40%
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0
期刊介绍: Chem Catalysis is a monthly journal that publishes innovative research on fundamental and applied catalysis, providing a platform for researchers across chemistry, chemical engineering, and related fields. It serves as a premier resource for scientists and engineers in academia and industry, covering heterogeneous, homogeneous, and biocatalysis. Emphasizing transformative methods and technologies, the journal aims to advance understanding, introduce novel catalysts, and connect fundamental insights to real-world applications for societal benefit.
期刊最新文献
Enhanced electrochemical reduction of CO2 to CO by ZnO nanorods enriched with oxygen vacancies Spatial effects define CO2 electrolysis systems Strong activity-based volcano-type relationship for dry reforming of methane through modulating Ni-CeO2 interaction over Ni/CeO2-SiO2 catalysts Cation effects on the alkaline oxygen reduction reaction Mechanistic insights into the electrochemical oxidation of acetate at noble metals
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