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Ni-based catalysts supported on Mg–Al hydrotalcites with different morphologies for CO2 methanation: exploring the effect of metal–support interaction
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020/02/25 , DOI: 10.1039/c9cy02523e Jie Ren 1, 2, 3, 4, 5 , Chalachew Mebrahtu 1, 2, 3, 4, 5 , Regina Palkovits 1, 2, 3, 4, 5
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2020/02/25 , DOI: 10.1039/c9cy02523e Jie Ren 1, 2, 3, 4, 5 , Chalachew Mebrahtu 1, 2, 3, 4, 5 , Regina Palkovits 1, 2, 3, 4, 5
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Metal oxide supported Ni-based catalysts represent intensively studied materials for CO2 methanation due to their relatively high activity, methane selectivity and low cost. However, the activity of Ni-based catalysts mainly depends on the nature of the used support during catalyst synthesis. Due to their good performance, hydrotalcite derived Mg–Al oxides have attracted significant attention as potential supports. However, the influence of support morphology on the active metal dispersion and catalytic performance has not yet been investigated. Hence, in order to study the effect of metal–support interaction, hydrotalcite derived Mg–Al supports with four different morphologies were designed and 20 wt% Ni was loaded as the active phase. The prepared materials were rigorously characterized by different techniques (XRD, SEM, FETEM, CO2-TPD, etc.) to study properties such as crystallite size, Ni dispersion, morphologies, and basic sites. The catalytic activity, selectivity and long-term stability of these four catalysts were evaluated for CO2 methanation (CO2 : H2 = 1 : 4) at different gas hourly space velocities, reaction temperatures, and reduction temperatures. Among the investigated catalysts, Ni/HT-10 i.e. 20 wt% Ni supported on the Mg–Al hydrotalcite with a “rosette-like” structure possesses superior CO2 conversion (83.5%), a TOF of 13.5 min−1 and 99.4% selectivity to CH4 at 400 °C. This superior catalytic activity results from its high basicity, optimized pore size, and defined support structure which lead to good Ni dispersion as well as a high exposed metallic surface area after reduction. Furthermore, Ni/HT-10 allowed stable catalytic activity for around 120 h on stream.
中文翻译：
镍基催化剂负载在具有不同形态的Mg-Al水滑石上以进行CO2甲烷化：探索金属与载体相互作用的影响
金属氧化物负载的镍基催化剂代表了对CO 2进行深入研究的材料甲烷化由于其相对较高的活性，甲烷选择性和低成本。但是，Ni基催化剂的活性主要取决于催化剂合成过程中所用载体的性质。由于其良好的性能，水滑石衍生的Mg-Al氧化物作为潜在的载体备受关注。然而，尚未研究载体形态对活性金属分散体和催化性能的影响。因此，为了研究金属-载体相互作用的影响，设计了具有四种不同形态的水滑石衍生的Mg-Al载体，并负载了20 wt％的Ni作为活性相。使用不同的技术（XRD，SEM，FETEM，CO 2 -TPD等）对制得的材料进行严格表征。）以研究诸如微晶尺寸，Ni分散度，形貌和碱性位点等性质。评价了这四种催化剂在不同的气体时空速，反应温度和还原温度下的CO 2甲烷化作用（CO 2 ：H 2 = 1：4）的催化活性，选择性和长期稳定性。在所研究的催化剂中，Ni / HT-10，即负载在具有“玫瑰花状”结构的Mg-Al水滑石上的20 wt％Ni具有优异的CO 2转化率（83.5％），TOF为13.5 min -1和99.4％对CH 4的选择性在400°C下。优异的催化活性归因于其高碱度，优化的孔径和确定的载体结构，可导致良好的Ni分散以及还原后的高暴露金属表面积。此外，Ni / HT-10允许在运行中约120小时保持稳定的催化活性。
更新日期：2020-03-26
中文翻译：
镍基催化剂负载在具有不同形态的Mg-Al水滑石上以进行CO2甲烷化：探索金属与载体相互作用的影响
金属氧化物负载的镍基催化剂代表了对CO 2进行深入研究的材料甲烷化由于其相对较高的活性，甲烷选择性和低成本。但是，Ni基催化剂的活性主要取决于催化剂合成过程中所用载体的性质。由于其良好的性能，水滑石衍生的Mg-Al氧化物作为潜在的载体备受关注。然而，尚未研究载体形态对活性金属分散体和催化性能的影响。因此，为了研究金属-载体相互作用的影响，设计了具有四种不同形态的水滑石衍生的Mg-Al载体，并负载了20 wt％的Ni作为活性相。使用不同的技术（XRD，SEM，FETEM，CO 2 -TPD等）对制得的材料进行严格表征。）以研究诸如微晶尺寸，Ni分散度，形貌和碱性位点等性质。评价了这四种催化剂在不同的气体时空速，反应温度和还原温度下的CO 2甲烷化作用（CO 2 ：H 2 = 1：4）的催化活性，选择性和长期稳定性。在所研究的催化剂中，Ni / HT-10，即负载在具有“玫瑰花状”结构的Mg-Al水滑石上的20 wt％Ni具有优异的CO 2转化率（83.5％），TOF为13.5 min -1和99.4％对CH 4的选择性在400°C下。优异的催化活性归因于其高碱度，优化的孔径和确定的载体结构，可导致良好的Ni分散以及还原后的高暴露金属表面积。此外，Ni / HT-10允许在运行中约120小时保持稳定的催化活性。
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