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Cooperation Between Active Metal and Basic Support in Ni-Based Catalyst for Low-Temperature CO2 Methanation
Catalysis Letters ( IF 2.8 ) Pub Date : 2019-11-13 , DOI: 10.1007/s10562-019-03033-w
Yuan Ma , Jiao Liu , Mo Chu , Junrong Yue , Yanbin Cui , Guangwen Xu

The key challenge for CO2 methanation, an eight-electron process under kinetic limitation, relies on the design of non-noble metal catalysts so as to achieve high activity at low reaction temperatures. In this work, four Ni-based catalysts with different supports were prepared and tested for CO2 methanation at 250–550 °C in a fixed bed quartz reactor and further characterized to reveal the structure–function relationship. The Ni-based catalysts followed an activity order of Ni/CeO2 > Ni/Al2O3 > Ni/TiO2 > Ni/ZrO2, especially at temperatures lower than 350 °C. H2-TPR and TPD results indicated that the interaction between nickel and support was strong and the metallic nickel was well dispersed in the Ni/Al2O3 catalyst, while more amount of CO2 was adsorbed on the weak basic sites in the Ni/CeO2 catalyst. By establishing the correlation between the catalytic performance and the catalyst structure, it was found that the Ni nanoparticles and basic support serve as H2 and CO2 active centers respectively and cooperatively catalyze CO2 methanation, resulting in high low-temperature reaction activity. High CO2 conversion was achieved over Ni/CeO2 catalyst at 300 °C for its high H2 uptake on Ni nanoparticles and high CO2 adsorption capacity on the support with weak basic sites and cooperatively to catalyze CO2 methanation.

中文翻译:

低温CO2甲烷化镍基催化剂中活性金属与碱性载体的合作

CO2 甲烷化是一种动力学限制下的八电子过程,其关键挑战依赖于非贵金属催化剂的设计,以便在低反应温度下实现高活性。在这项工作中,制备了四种不同载体的镍基催化剂,并在固定床石英反应器中在 250-550°C 下测试了 CO2 甲烷化,并进一步表征以揭示结构 - 功能关系。镍基催化剂的活性顺序为 Ni/CeO2 > Ni/Al2O3 > Ni/TiO2 > Ni/ZrO2,尤其是在低于 350 °C 的温度下。H2-TPR和TPD结果表明镍和载体之间的相互作用很强,金属镍在Ni/Al2O3催化剂中分散良好,而更多的CO2吸附在Ni/CeO2催化剂的弱碱性位点上。通过建立催化性能与催化剂结构之间的相关性,发现Ni纳米颗粒和基础载体分别作为H2和CO2活性中心,协同催化CO2甲烷化,具有较高的低温反应活性。Ni/CeO2 催化剂在 300°C 下实现了高 CO2 转化率,因为它在 Ni 纳米颗粒上的高 H2 吸收和在具有弱碱性位点的载体上的高 CO2 吸附能力,并协同催化 CO2 甲烷化。
更新日期:2019-11-13
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